One-Step Multipurpose Surface Functionalization by Adhesive Catecholamine.
Kang Sung Min,Hwang Nathaniel S,Yeom Jihyeon,Park Sung Young,Messersmith Phillip B,Choi Insung S,Langer Robert,Anderson Daniel G,Lee Haeshin
Advanced functional materials
Surface modification is one of the most important techniques in modern science and engineering. The facile introduction of a wide variety of desired properties onto virtually any material surface is an ultimate goal in surface chemistry. To achieve this goal, the incorporation of structurally diverse molecules onto any material surface is an essential capability for ideal surface modification. Here, we present a general strategy of surface modification, in which many diverse surfaces can be functionalized by immobilizing a wide variety of molecules. This strategy functionalizes surfaces by a one-step immersion of substrates in a one-pot mixture of a molecule and a catecholamine surface modification agent. This one-step procedure for surface modification represents a standard protocol to control interfacial properties.
Three-dimensional electrospun nanofibrous scaffolds displaying bone morphogenetic protein-2-derived peptides for the promotion of osteogenic differentiation of stem cells and bone regeneration.
Ye Kaiqiang,Liu Dinghua,Kuang Haizhu,Cai Jiangyu,Chen Weiming,Sun Binbin,Xia Lunguo,Fang Bing,Morsi Yosry,Mo Xiumei
Journal of colloid and interface science
Tissue scaffolds with three-dimensional (3D) nanofibrous biomimetic structures have attracted attention in the field of bone regeneration. In recent years, emerging strategies based on electrospinning technologies have facilitated the preparation of 3D nanofibrous scaffolds. Based on these developments, in this study, 3D scaffolds possessing both nanofibrous morphologies and interconnected pores were fabricated for their potential in bone tissue engineering. By combining homogenizing, freeze-drying, and thermal crosslinking techniques, nano-hydroxyapatite/PLLA/gelatin (nHA/PLA/GEL) 3D nanofibrous scaffolds were prepared using pre-fabricated electrospun nanofibers. Then, utilizing a polydopamine (pDA)-assisted coating strategy, bone morphogenetic protein-2 (BMP-2)-derived peptides were further immobilized onto the 3D scaffolds to obtain the resulting nano-hydroxyapatite/PLLA/gelatin-peptide (nHA/PLA/GEL-PEP) 3D nanofibrous scaffolds capable of sustained release. Bone mesenchymal stem cells (BMSCs) were cultured on the 3D nanofibrous scaffolds, then relative cell viability, alkaline phosphatase (ALP) activity, and gene expression assays were performed to study the effects of the scaffolds on cell growth and osteogenic differentiation in vitro. Furthermore, the ability of bone formation in vivo was evaluated using a rat cranial bone defect model. In vitro and in vivo results demonstrated that the 3D nanofibrous scaffolds incorporated with nHA and BMP-2 peptides exhibited favorable biocompatibility and osteoinductivity. Therefore, these nanofibrous scaffolds have excellent potential in bone regenerative medicine.
Hydroxyapatite/silver electrospun fibers for anti-infection and osteoinduction.
Liu Feifei,Wang Xiaohui,Chen Tongtong,Zhang Naiyin,Wei Qin,Tian Juling,Wang Yingbo,Ma Chuang,Lu Yong
Journal of advanced research
Bone implant materials cause the most common complication of bone infections in orthopedic surgery, resulting in implant failure. Antibiotic treatment of bone infections leads to problems such as bacterial resistance and reduced osteogenic capacity. In this study, dopamine (DA) was self-polymerized on the surface of Polylactic acid (PLLA)/Hydroxyapatite (HA) nanowire composite fibers to form an adhesive polydopamine (PDA) membrane, and a stable silver-nanoparticles (Ag-NPs) coating layer was constructed on it by electrochemically driven Ag coordination and chelation through Polypyrrole (PPy) mediation, achieving steady and slow release of Ag-NPs. With optimized DA soaking time of 24 h and soaking concentration of 0.5 g·L, nanoparticles were uniformly distributed on PLLA/HA/PDA/PPy/Ag composite fibers and the hydrophilicity of the composite fibers was well-behaved. Besides, the composite fibers possessed good physiological stability and 100% antibacterial rate against () as well as (). In addition, the composite fibers had promoted apatite nucleation and growth on surface and good cytocompatibility with osteoblasts, indicating ability of inducing osteogenic differentiation. In summary, a multi-functional PLLA/HA/PDA/PPy/Ag composite fiber with long-term antibacterial property, bioactivity and osteoinductivity was successfully constructed by electrospinning and electrochemical deposition.
Triple-Bioinspired Burying/Crosslinking Interfacial Coassembly Strategy for Layer-by-Layer Construction of Robust Functional Bioceramic Self-Coatings for Osteointegration Applications.
Jia Zhaojun,Xiu Peng,Roohani-Esfahani Seyed-Iman,Zreiqat Hala,Xiong Pan,Zhou Wenhao,Yan Jianglong,Cheng Yan,Zheng Yufeng
ACS applied materials & interfaces
Coating bioceramics of inherent bioactivity onto biometallic implants is a straightforward yet promising solution to address poor osteointegration of the latter. One step further, it would be a nontrivial accomplishment to develop a mild, cheap, and universal route to firmly stabilizing, in principle, any ceramics onto any implant substrate, while imparting expectedly versatile biofunctional performances. Herein, we describe a triple-bioinspired burying/cross-linking interfacial coassembly strategy for enabling such ceramic coatings, which ingeniously fuses bioinspiration from sea rocks (burying assisted particle immobilization), marine mussels (universal adhesion and versatile chemical reactivity), and reef-building oysters (cross-linking rendered cohesion). Specifically, surface functionalized, aqueous dispersed ceramic particles were buried within an substrate-anchored organic matrix of polyelectrolyte multilayers (i.e., (poly(ether imide) (PEI)/poly(sodium-p-styrenesulfonate) (PSS)) ), through a new inorganic-organic hybrid layer-by-layer (LBL) coassembly scheme wherein mussel (oyster) inspired adhesive (cohesive) chemistries were exquisitely orchestrated. As a conceptual demonstration, bioactive baghdadite (CaZrSiO) was synthesized as model ceramics, with which we constructed on medical titanium robust, biomimetic, and cross-linkable LBL self-assemblies harnessing the said strategy. Intimate substrate contacts and well-defined buried inorganic-organic interfaces were evidently seen, together with good structural and chemical stabilities, especially after cross-linking. Sustained bioactive ion releasing and appreciable biomineralization activity were confirmed in vitro. Subsequently, biological performances of the assemblies were systematically investigated with respect to surface hydrophilicity, protein adsorption, and osteoblast functions. Additionally, nanosilver deposition, which imparted the surfaces with added antibacterial potencies, was used to exemplify the strategy's versatility in allowing multifunctionality. What's more, the flexibility of our approach was testified through modifying clinically relevant complicated 3D porous scaffolds. Overall, our strategy basically met the design expectations, boding well for future medical adoption. This study offers the promise of an alternative broadly useful avenue to bioactive and functional surface design of bone implants. It may also provide insights into other multiple-bioinspired materials/interfaces for biological and other applications.
In Situ Bone Tissue Engineering With an Endogenous Stem Cell Mobilizer and Osteoinductive Nanofibrous Polymeric Scaffolds.
Lee Jong Seung,Jin Yoonhee,Park Hyun-Ji,Yang Kisuk,Lee Min Suk,Yang Hee Seok,Cho Seung-Woo
Classical bone tissue engineering involves the use of culture-expanded cells and scaffolds to produce tissue constructs for transplantation. Despite promising results, clinical adoption of these constructs has been limited due to various drawbacks, including extensive cell expansion steps, low cell survival rate upon transplantation, and the possibility of immuno-rejection. To bypass the ex vivo cell culture and transplantation process, the regenerative capacity of the host is exploited by mobilizing endogenous stem cells to the site of injury. Systemic injection of substance P (SP) induce mobilization of CD29 CD105 CD45 cells from bone marrow and enhance bone tissue regeneration in a critical-sized calvarial bone defect model. To provide an appropriate environment for endogenous stem cells to survive and differentiate into osteogenic lineage cells, electrospun nanofibrous polycaprolactone (PCL) scaffolds are functionalized with hydroxyapatite (HA) particles via a polydopamine (PDA) coating to create highly osteoinductive PCL-PDA-HA scaffolds that are implanted in defects. The combination of the PCL-PDA-HA scaffold and SP treatment enhance in situ bone tissue formation in defects. Thus, this in situ bone regeneration strategy, which combines recruitment of endogenous stem cells from the bone marrow to defective sites and implantation of a highly biocompatible and osteoinductive cell-free scaffold system, has potential as an effective therapeutic in regenerative medicine.
Mussel-inspired dual-functional PEG hydrogel inducing mineralization and inhibiting infection in maxillary bone reconstruction.
Xu Huiyong,Zhang Ge,Xu Kaige,Wang Leyu,Yu Lei,Xing Malcolm M Q,Qiu Xiaozhong
Materials science & engineering. C, Materials for biological applications
Infection compromises healing process after bone fracture. An anti-bacterial bone graft synthesized from polymer and mineralization components is becoming preferable for its accessibility and low cost and tunable chem-physic properties. In this study, mussel-inspired polydopamine (PDA) was used to synthesize in-situ silver nanoparticles (AgNPs) and mineralization on polyethylene hydrogel (PEG). With dual functions of anti-bacteria and graft mineralization, we found the hydrogel (AgNPs/PDA) promoted bone generation and show significant antibacterial activity. Specifically, the gel upregulated the expression of osteogenic genes of bone sialoprotein gene, alkaline phosphatase, osteocalcin and runt-related transcription factor 2. It also significantly inhibited the growth of Staphylococcus aureus and Escherichia coli. In vivo the AgNPs/PDA gel could repair maxillary bone defect efficiently.
Development of mussel-inspired 3D-printed poly (lactic acid) scaffold grafted with bone morphogenetic protein-2 for stimulating osteogenesis.
Cheng Cheng-Hsin,Chen Yi-Wen,Kai-Xing Lee Alvin,Yao Chun-Hsu,Shie Ming-You
Journal of materials science. Materials in medicine
3D printing is a versatile technique widely applied in tissue engineering due to its ability to manufacture large quantities of scaffolds or constructs with various desired architectures. In this study, we demonstrated that poly (lactic acid) (PLA) scaffolds fabricated via fused deposition not only retained the original interconnected microporous architectures, the scaffolds also exhibited lower lactic acid dissolution as compared to the freeze-PLA scaffold. The 3D-printed scaffolds were then grafted with human bone morphogenetic protein-2 (BMP-2) via the actions of polydopamine (PDA) coatings. The loading and release rate of BMP-2 were monitored for a period of 35 days. Cellular behaviors and osteogenic activities of co-cultured human mesenchymal stem cells (hMSCs) were assessed to determine for efficacies of scaffolds. In addition, we demonstrated that our fabricated scaffolds were homogenously coated with PDA and well grafted with BMP-2 (219.1 ± 20.4 ng) when treated with 250 ng/mL of BMP-2 and 741.4 ± 127.3 ng when treated with 1000 ng/mL of BMP-2. This grafting enables BMP-2 to be released in a sustained profile. From the osteogenic assay, it was shown that the ALP activity and osteocalcin of hMSCs cultured on BMP-2/PDA/PLA were significantly higher when compared with PLA and PDA/PLA scaffolds. The methodology of PDA coating employed in this study can be used as a simple model to immobilize multiple growth factors onto different 3D-printed scaffold substrates. Therefore, there is potential for generation of scaffolds with different unique modifications with different capabilities in regulating physiochemical and biological properties for future applications in bone tissue engineering.
Deposition Kinetics of Bioinspired Phenolic Coatings on Titanium Surfaces.
Geißler Sebastian,Barrantes Alejandro,Tengvall Pentti,Messersmith Phillip B,Tiainen Hanna
Langmuir : the ACS journal of surfaces and colloids
Polyphenols can form functional coatings on a variety of different materials through auto-oxidative surface polymerization in a manner similar to polydopamine coatings. However, the mechanisms behind the coating deposition are poorly understood. We report the coating deposition kinetics of the polyphenol tannic acid (TA) and the simple phenolic compound pyrogallol (PG) on titanium surfaces. The coating deposition was followed in real time over a period of 24 h using a quartz crystal microbalance with dissipation monitoring (QCM-D). TA coatings revealed a multiphasic layer formation: the deposition of an initial rigid layer was followed by the buildup of an increasingly dissipative layer, before mass adsorption stopped after approximately 5 h of coating time. The PG deposition was biphasic, starting with the adsorption of a nonrigid viscoelastic layer which was followed by layer stiffening upon further mass adsorption. Coating evaluation by ellipsometry and AFM confirmed the deposition kinetics determined by QCM-D and revealed maximum coating thicknesses of approximately 50 and 75 nm for TA and PG, respectively. Chemical characterization of the coatings and polymerized polyphenol particles indicated the involvement of both physical and chemical interactions in the auto-oxidation reactions.
Advances in functionalized polymer coatings on biodegradable magnesium alloys - A review.
Li Ling-Yu,Cui Lan-Yue,Zeng Rong-Chang,Li Shuo-Qi,Chen Xiao-Bo,Zheng Yufeng,Kannan M Bobby
Magnesium (Mg) and its alloys have become a research frontier in biodegradable materials owing to their superior biocompatibility and excellent biomechanical compatibility. However, their high degradation rate in the physiological environment should be well tackled prior to clinical applications. This review summarizes the latest progress in the development of polymeric coatings on biodegradable Mg alloys over the last decade, regarding preparation strategies for polylactic acid (PLA), poly (latic-co-glycolic) acid (PLGA), polycaprolactone (PCL), polydopamine (PDA), chitosan (CS), collagen (Col) and their composite, and their performance in terms of corrosion resistance and biocompatibility. Feasible perspectives and developing directions of next generation of polymeric coatings with respect to biomedical Mg alloys are briefly discussed. STATEMENT OF SIGNIFICANCE:Magnesium (Mg) and its alloys have become a research frontier in biodegradable materials owing to their superior biocompatibility and suitable biomechanical compatibility. However, the principal drawback of Mg-based implants is their poor corrosion resistance in physiological environments. Hence, it is vital to mitigate the degradation/corrosion behavior of Mg alloys for safe biomedical deployments. This review summarizes the latest progress in development of polymeric coatings on biomedical Mg alloys regarding preparation strategy, corrosion resistance and biocompatibility, including polylactic acid (PLA), poly (latic-co-glycolic) acid (PLGA), polycaprolactone (PCL), chitosan (CS), polydopamine (PDA), collagen (Col) and their composite. In addition, functionalized polymer coatings with Mg alloys exhibits a promising prospect owing to their ability of degradation along with biocompatibility, self-healing, drug-delivery and osteoinduction.
Influence of Mussel-Derived Bioactive BMP-2-Decorated PLA on MSC Behavior in Vitro and Verification with Osteogenicity at Ectopic Sites in Vivo.
Chen Zhuoyue,Zhang Zhen,Feng Juantao,Guo Yayuan,Yu Yuan,Cui Jihong,Li Hongmin,Shang Lijun
ACS applied materials & interfaces
Osteoinductive activity of the implant in bone healing and regeneration is still a challenging research topic. Therapeutic application of recombinant human bone morphogenetic protein-2 (BMP-2) is a promising approach to enhance osteogenesis. However, high dose and uncontrolled burst release of BMP-2 may introduce edema, bone overgrowth, cystlike bone formation, and inflammation. In this study, low-dose BMP-2 of 1 μg was used to design PLA-PD-BMP for functionalization of polylactic acid (PLA) implants via mussel-inspired polydopamine (PD) assist. For the first time, the binding property and efficiency of the PD coating with BMP-2 were directly demonstrated and analyzed using an antigen-antibody reaction. The obtained PLA-PD-BMP surface immobilized with this low BMP-2 dose can endow the implants with abilities of introducing strong stem cell adhesion and enhanced osteogenicity. Furthermore, in vivo osteoinduction of the PLA-PD-BMP-2 scaffolds was confirmed by a rat ectopic bone model, which is marked as the "gold standard" for the evidence of osteoinductive activity. The microcomputed tomography, Young's modulus, and histology analyses were also employed to demonstrate that PLA-PD-BMP grafted with 1 μg of BMP-2 can induce bone formation. Therefore, the method in this study can be used as a model system to immobilize other growth factors onto various different types of polymer substrates. The highly biomimetic mussel-derived strategy can therefore improve the clinical outcome of polymer-based medical implants in a facile, safe, and effective way.
Strategic design of a Mussel-inspired in situ reduced Ag/Au-Nanoparticle Coated Magnesium Alloy for enhanced viability, antibacterial property and decelerated corrosion rates for degradable implant Applications.
Rezk Abdelrahman I,Ramachandra Kurup Sasikala Arathyram,Nejad Amin Ghavami,Mousa Hamouda M,Oh Young Min,Park Chan Hee,Kim Cheol Sang
Magnesium (Mg) and its alloys have attracted much attention as a promising candidate for degradable implant applications however the rapid corrosion of magnesium inside the human body greatly limits its use as an implant material. Therefore, coating the alloy surface with a multifunctional film is a promising way to overcome the drawbacks. Here we propose for the first time a multifunction layer coating to enhance the cell viability, antibacterial property and decelerated corrosion rates to act as a novel material to be used for degradable implant Applications. For that, the magnesium alloy (AZ31) was first treated with hydrofluoric acid (HF) and then dopamine tris Hydrochloric acid (tris-HCL) solution. The reducing catechol groups in the polydopamine (PD) layer subsequently immobilize silver/gold ions in situ to form uniformly dispersed Ag/Au nanoparticles on the coating layer. The successful formation of Ag/Au nanoparticles on the HF-PD AZ31 alloy was confirmed using XPS and XRD, and the morphology of all the coated samples were investigated using SEM images. The alloy with HF-PDA exhibit enhanced cell attachment and proliferation. Moreover, the nanoparticle immobilized HF-PD alloy exhibited dramatic corrosion resistance enhancement with superior antibacterial properties and accountable biocompatibility. Thus the result suggest that HF-PD Ag/Au alloy has great potential in the application of degradable implant and the surface modification method is of great significance to determine its properties.
Poly(dopamine) and Ag nanoparticle-loaded TiO nanotubes with optimized antibacterial and ROS-scavenging bioactivities.
Gao Chenghao,Cheng Hao,Xu Na,Li Yong,Chen Yangmengfan,Wei Yong,Gao Biao,Fu Jijiang,Huo Kaifu,Xiong Wei
Nanomedicine (London, England)
AIM:To create polydopamine (PDA) and Ag nanoparticle-loaded TiO nanotubes coating on titanium (Ti) alloy. MATERIALS & METHODS:TiO-PDA-Ag coating was fabricated on Ti implants by electrochemical anodization. The in vitro and in vivo bactericidal and antibiofilm activities were tested. Intracellular reactive oxygen species (ROS) and antioxidative capability were measured, and cell proliferation, adhesion and cell morphology were characterized. RESULTS:TiO-PDA-Ag coating showed satisfactory bactericidal and antibiofilm activities in vitro and in vivo, improved Ag release pattern, evident ROS scavenging properties and enhanced cell adhesion and proliferation. CONCLUSION:Our study successfully fabricated a PDA and Ag nanoparticle-loaded TiO nanotubes coating on Ti alloy. The improved Ag release kinetics and ROS-scavenging properties achieve an optimal balance between antibacterial ability and biocompatibility.
The relationship between substrate morphology and biological performances of nano-silver-loaded dopamine coatings on titanium surfaces.
Zhang Weibo,Wang Shuang,Ge Shaohua,Chen Jialong,Ji Ping
Royal Society open science
Biomedical device-associated infection (BAI) and lack of osseointegration are the main causes of implant failure. Therefore, it is imperative for implants not only to depress microbial activity and biofilm colonization but also to prompt osteoblast functions and osseointegration. As part of the coating development for implants, the interest of studies on the interaction between implant substrate morphology and the coating's biological performances is growing. In this study, by harnessing the adhesion and reactivity of bioinspired polydopamine, nano-silver was successfully anchored onto micro/nanoporous as well as smooth titanium surfaces to analyse the effect of substrate morphology on biological performances of the coatings. Compared with the smooth surface, a small size of nano-silver and high silver content was found on the micro/nanoporous surface. More mineralization happened on the coating on the micro/nanoporous structure than on the smooth surface, which led to a more rapid decrease of silver release from the micro/nanoporous surface. Antimicrobial tests indicated that both surfaces with resulting coating inhibit microbial colonization on them and growth around them, indicating that the coating eliminates the shortcoming of the porous structure which render the implant extremely susceptible to BAI. Besides, the multiple osteoblast responses of nano-silver-loaded dopamine coatings on both surfaces, i.e. attachment, proliferation and differentiation, have deteriorated, however the mineralized surfaces of these coatings stimulated osteoblast proliferation and differentiation, especially for the micro/nanoporous surface. Therefore, nano-silver-loaded dopamine coatings on micro/nanoporous substratum may not only reduce the risk of infection but also facilitate mineralization during the early post-operative period and then promote osseointegration owing to the good osteoblast-biocompatibility of the mineralized surface. These results clearly highlight the influence of the substrate morphology on the biological performances of implant coating.
Surface functionalization of polytetrafluoroethylene substrate with hybrid processes comprising plasma treatment and chemical reactions.
Cheng Bohan,Inoue Yuuki,Ishihara Kazuhiko
Colloids and surfaces. B, Biointerfaces
Polytetrafluoroethylene (PTFE) exhibits excellent mechanical properties and chemical stability and has been widely used in medical fields for the preparation of implantable medical devices. However, the implantation of PTFE in living systems results in inflammation reactions and infections at the surface thus limits its long-term applications. For PTFE surface modification, we examined the effects of mussel-inspired polydopamine (PDA) coating and the further introduction of functional groups. During PDA coating, the plasma pretreatment on PTFE enhanced the stability of the PDA coating layer. Furthermore, the introduction of functional groups on the PDA layer was carried out using reactive functional groups for the photoinduced graft polymerization of methacrylate. For instance, 2-methacryloyloxyethyl phosphorylcholine (MPC) could be polymerized from the surface of the substrate. These chemical modifications were confirmed step by step using spectroscopes to obtain the hydrophilic surface of the poly(MPC)-modified PTFE. The protein adsorption behaviors on PTFE and poly(MPC)-modified PTFE were compared to understand biocompatibility characteristics of these substrates. The surface of PTFE was immediately covered with albumin and the contact between the substrate and the serum resulted in an increase in the fibrinogen composition with time. On the other hand, fewer proteins were adsorbed on the poly(MPC)-modified PTFE substrate. Thus, this modification procedure would serve as a strategy for safer alterations in PTFE surfaces to expand the life span of the PTFE-carrying medical devices in living systems.
Mineral Trioxide Aggregate with Mussel-inspired Surface Nanolayers for Stimulating Odontogenic Differentiation of Dental Pulp Cells.
Tu Ming-Gene,Ho Chia-Che,Hsu Tuan-Ti,Huang Tsui-Hsien,Lin Min-Jhen,Shie Ming-You
Journal of endodontics
INTRODUCTION:This research was intended to evaluate the feasibility of mineral trioxide aggregate (MTA) powder coated with polydopamine (PDA) in dental and bone tissue regeneration by investigating the hydration, physicochemical properties, and biological performance of hydrated cements. METHODS:The MTA powder was well suspended in a dopamine solution buffered at a pH of 8.5 using tris(hydroxymethyl)aminomethane buffer and vigorously stirred for 12 hours at room temperature. The PDA-coated MTA powder was mixed with water and hydrated at 37°C with 100% relative humidity for 1 day. The setting time, mechanical strength, phase composition, surface morphology, and in vitro bioactivity of the cements as well as the proliferation and odontogenic differentiation of human dental pulp cells cultured on the cements were evaluated. RESULTS:The setting of the MTA cements was significantly shortened without jeopardizing the mechanical properties with PDA incorporated into the cements. In addition, our results proved that PDA-coated MTA up-regulation of odontogenic-related protein of hDPCs. PDA-coated MTA induced the odontogenic differentiation of cells as indicated by an alkaline phosphate activity test and an odontogenic-related protein analysis. CONCLUSIONS:These results indicate that dopamine is an effective coating material to promote long-term human dental pulp cell culture and odontogenic differentiation on PDA-MTA substrates. This will be an important direction for future studies focused on developing new biomaterials for dental applications.
One-Step Coating toward Multifunctional Applications: Oil/Water Mixtures and Emulsions Separation and Contaminants Adsorption.
Cao Yingze,Liu Na,Zhang Weifeng,Feng Lin,Wei Yen
ACS applied materials & interfaces
Here, a method that can simultaneously separate oil/water mixtures and remove water-soluble contaminants has been developed. Various substrates with different pore size were coated by polydopamine and polyethylenepolyamine codeposition films. The as-prepared materials were superhydrophilic and under-water superoleophobic. The materials can separate a range of different oil/water mixtures (including immiscible oil/water mixtures and surfactant-stabilized emulsions) in a single unit operation, with >99.6% separation efficiency and high fluxes. Copper ion and methyl blue can be effectively absorbed from water when it permeates through the materials. This method can be applied on organic and inorganic substrates and used in preparing large-scale product. Therefore, the simple and facile method has excellent potential in practical application and creates a new field for oil/water separation materials with multifunctional applications.
Poly(2-oxazoline)s One-Pot Polymerization and Surface Coating: From Synthesis to Antifouling Properties Out-Performing Poly(ethylene oxide).
Svoboda Jan,Sedláček Ondřej,Riedel Tomáš,Hrubý Martin,Pop-Georgievski Ognen
Poly(2-alkyl-2-oxazoline)s (PAOx) represent a class of emerging polymers that can substitute or even outperform poly(ethylene oxide) (PEO) standard in various applications. Despite the great advances in PAOx research, there is still a gap in the direct experimental comparison of antifouling properties between PAOx and the golden standard PEO when exposed to blood. Motivated by this, we developed a straightforward protocol for the one-pot PAOx polymerization and surface coating by a "grafting to-" approach. First, we synthesized a library of hydrophilic poly(2-methyl-2-oxazoline)s (PMeOx) and poly(2-ethyl-2-oxazoline)s (PEtOx) with molar mass ranging from 1.5 to 10 kg/mol (DP = 16-115). The PAOx living chains were directly terminated by amine and hydroxyl groups of polydopamine (PDA) anchor layer providing the highest so far reported grafting densities ranging from 0.2 to 2.1 chains/nm. In parallel, PEO chains providing the same degree of polymerization (molar mass from 1.2 to 5 kg/mol, DP = 28-116) bearing thiol groups were grafted to PDA. The thickness, surface-related parameters, covalent structure, and antifouling properties of the resulting polymer brushes were determined via various surface sensitive techniques. The comparison of the synthesized PAOx and PEO brushes led us to the conclusion that at the same surface-related parameters, PMeOx brushes show significantly better antifouling character when challenged against human blood plasma.
Poly(Dopamine) Coating on 3D-Printed Poly-Lactic-Co-Glycolic Acid/β-Tricalcium Phosphate Scaffolds for Bone Tissue Engineering.
Xu Zhimin,Wang Ningning,Liu Peng,Sun Yidan,Wang Yumeng,Fei Fan,Zhang Shichen,Zheng Jianying,Han Bing
Molecules (Basel, Switzerland)
Bone defects caused by osteoporosis, bone malignant tumors, and trauma are very common, but there are many limiting factors in the clinical treatment of them. Bone tissue engineering is the most promising treatment and is considered to be the main strategy for bone defect repair. We prepared polydopamine-coated poly-(lactic-co-glycolic acid)/β-tricalcium phosphate composite scaffolds via 3D printing, and a series of characterization and biocompatibility tests were carried out. The results show that the mechanical properties and pore-related parameters of the composite scaffolds are not affected by the coatings, and the hydrophilicities of the surface are obviously improved. Scanning electron microscopy and micro-computed tomography display the nanoscale microporous structure of the bio-materials. Biological tests demonstrate that this modified surface can promote cell adhesion and proliferation and improve osteogenesis through the increase of polydopamine (PDA) concentrations. Mouse cranial defect experiments are conducted to further verify the conclusion that scaffolds with a higher content of PDA coatings have a better effect on the formation of new bones. In the study, the objective of repairing critical-sized defects is achieved by simply adding PDA as coatings to obtain positive results, which can suggest that this modification method with PDA has great potential.
Triple PLGA/PCL Scaffold Modification Including Silver Impregnation, Collagen Coating, and Electrospinning Significantly Improve Biocompatibility, Antimicrobial, and Osteogenic Properties for Orofacial Tissue Regeneration.
Qian Yunzhu,Zhou Xuefeng,Zhang Feimin,Diekwisch Thomas G H,Luan Xianghong,Yang Jianxin
ACS applied materials & interfaces
Biodegradable synthetic scaffolds hold great promise for oral and craniofacial guided tissue regeneration and bone regeneration. To overcome the limitations of current scaffold materials in terms of osteogenic and antimicrobial properties, we have developed a novel silver-modified/collagen-coated electrospun poly-lactic-co-glycolic acid/polycaprolactone (PLGA/PCL) scaffold (PP-pDA-Ag-COL) with improved antimicrobial and osteogenic properties. Our novel scaffold was generated by electrospinning a basic PLGA/PCL matrix, followed by silver nanoparticles (AgNPs) impregnation via in situ reduction, polydopamine coating, and then coating by collagen I. The three intermediate materials involved in the fabrication of our scaffolds, namely, PLGA/PCL (PP), PLGA/PCL-polydopamine (PP-pDA), and PLGA/PCL-polydopamine-Ag (PP-pDA-Ag), were used as control scaffolds. Scanning electron micrographs and mechanical testing indicated that the unique three-dimensional structures with randomly oriented nanofibrous electrospun scaffold architectures, the elasticity modulus, and the tensile strength were maintained after modifications. CCK-8 cell proliferation analysis demonstrated that the PP-pDA-Ag-COL scaffold was associated with higher MC3T3 proliferation rates than the three control scaffolds employed. Scanning electron and fluorescence light microscopy illustrated that PP-pDA-Ag-COL scaffolds significantly enhanced MC3T3 cell adhesion compared to the control scaffolds after 12 and 24 h culture, in tandem with the highest β1 integrin expression levels, both at the mRNA level and the protein level. Alkaline phosphatase activity, BMP2, and RUNX2 expression levels of MC3T3 cells cultured on PP-pDA-Ag-COL scaffolds for 7 and 14 days were also significantly higher when compared to controls ( < 0.001). There was a wider antibacterial zone associated in PP-pDA-Ag-COL and PP-pDA-Ag scaffolds versus control scaffolds ( < 0.05), and bacterial fluorescence was reduced on the Ag-modified scaffolds after 24 h inoculation against and . In a mouse periodontal disease model, the PP-pDA-Ag-COL scaffold enhanced alveolar bone regeneration (31.8%) and was effective for periodontitis treatment. These results demonstrate that our novel PP-pDA-Ag-COL scaffold enhanced biocompatibility and osteogenic and antibacterial properties and has therapeutic potential for alveolar/craniofacial bone regeneration.
In Situ Polymerization of Dopamine on Graphene Framework for Charge Storage Applications.
Liu Tianyuan,Lee Byeongyong,Kim Byoung Gak,Lee Michael J,Park Jinho,Lee Seung Woo
Small (Weinheim an der Bergstrasse, Germany)
Polydopamine, a functional coating material, is redox active as cathode materials for both Li- and Na-ion batteries or hybrid capacitors. Here, a polydopamine coating onto 3D graphene framework is introduced through a simple hydrothermal process, during which graphene oxide serves not only as an oxidant for assisting the polymerization of dopamine, but also as a template for the conformal growth of polydopamine. High-density films are fabricated by compressing the polydopamine-coated graphene aerogels, which can be directly used as free-standing and flexible cathodes in both Li- and Na-cells. The compact electrodes deliver high capacities of ≈230 mAh g in Li-cells and ≈211 mAh g in Na-cells based on the total mass of electrodes. These compact electrodes also exhibit exceptional cycling stability and high rate performance due to the unique structure in which polydopamine is uniformly coated on the 3D structured graphene.
Controlled Retention of BMP-2-Derived Peptide on Nanofibers Based on Mussel-Inspired Adhesion for Bone Formation.
Lee Jinkyu,Perikamana Sajeesh Kumar Madhurakkat,Ahmad Taufiq,Lee Min Suk,Yang Hee Seok,Kim Do-Gyoon,Kim Kyobum,Kwon Bosun,Shin Heungsoo
Tissue engineering. Part A
Although bone morphogenetic protein-2 (BMP-2) has been frequently used to stimulate bone formation, it has several side effects to be addressed, including the difficulty in optimization of clinically relevant doses and unwanted induction of cancerous signaling processes. In this study, an osteogenic peptide (OP) derived from BMP-2 was investigated as a substitute for BMP-2. In vitro studies showed that OP was able to enhance the osteogenic differentiation and mineralization of human mesenchymal stem cells (hMSCs). The peptides were then conjugated onto biocompatible poly-ι-lactide electrospun nanofibers through polydopamine chemistry. Surface chemical analysis proved that more than 80% of the peptides were stably retained on the nanofiber surface after 8 h of polydopamine coating during at least 28 days, and the amount of peptides that was retained increased depending on the polydopamine coating time. For instance, about 65% of the peptides were retained on nanofibers after 4 h of polydopamine coating. Also, a relatively small dose of peptides could effectively induce bone formation in in vivo critical-sized defects on the calvarial bones of mice. More than 50.4% ± 16.9% of newly formed bone was filled within the defect after treatment with only 10.5 ± 0.6 μg of peptides. Moreover, these groups had similar elastic moduli and contact hardnesses with host bone. Taken together, our results suggest that polydopamine-mediated OP immobilized on nanofibers can modulate the retention of relatively short lengths of peptides, which might make this an effective therapeutic remedy to guide bone regeneration using a relatively small amount of peptides.
Polydopamine as a stable and functional nanomaterial.
El Yakhlifi Salima,Ball Vincent
Colloids and surfaces. B, Biointerfaces
The mussel inspired chemistry of dopamine leading to versatile coatings on the surface of all kinds of materials in a one pot process was considered as the unique aspect of catecholamine for a long time. Only recently, research has been undertaken to valorize the simultaneous oxidation and colloid formation in dopamine solutions in the presence of an oxidant. This mini review summarizes the synthesis methods allowing to get controlled nanomaterials, either nanoparticles, hollow capsules or nanotubes and even chiral nanomaterials from dopamine solutions. Finally the applications of those nanomaterials will be described.
One-Pot UV-Triggered o-Nitrobenzyl Dopamine Polymerization and Coating for Surface Antibacterial Application.
Shi Liya,Santhanakrishnan Sridhar,Cheah Yong Shung,Li Min,Chai Christina Li Lin,Neoh Koon Gee
ACS applied materials & interfaces
Dopamine (DA) protected by an o-nitrobenzyl functionality on its phenolic group was synthesized as a photolabile catecholamine derivative. This compound, o-nitrobenzyl dopamine (NBDA), was more stable than DA in basic solution at pH 8.5 and will not self-polymerize when protected from light. UV irradiation of a methanolic solution of NBDA at 365 nm for 40 min induced ca. 85% deprotection. Taking advantage of the stability of NBDA, a one-pot spray coating technique for modifying surfaces with polydopamine (PDA) was developed. Using ethylene glycol with Tris buffer (pH 8.5) as the solvent for this technique, stainless steel substrates can be coated with a robust PDA layer. Silver was deposited on the PDA-coated surface after treatment with silver nitrate solution, and >80% of the deposited silver remained on the surface after 1 week immersion in water. The NBDA-Ag surface was highly effective in inhibiting Staphylococcus aureus (S. aureus) biofilm formation.
Polydopamine modification of silk fibroin membranes significantly promotes their wound healing effect.
Zhang Ying,Lu Leihao,Chen Yuping,Wang Jie,Chen Yuyin,Mao Chuanbin,Yang Mingying
Natural polymer-based wound dressings have gained great attention in skin tissue engineering. Silk fibroin (SF) spun from Bombyx mori (B. mori) is a potential wound dressing material due to its outstanding biocompatibility and biodegradability, however, its wound healing effect is still limited. To maximize the wound healing effect of SF-based wound dressing, we first fabricated fibrous electrospun SF (ESF) membranes with large porosity and specific surface area, and then formed polydopamine (PDA) coating on the ESF fibers to form PESF membranes. We found that PDA coating enabled the PESF membranes to outperform the ESF membranes in enhancing the hydrophilicity and protein adsorption ability of the membranes as well as the attachment, spreading and proliferation of fibroblasts on the membranes in vitro. Our further in vivo histological analysis confirmed that the PESF membranes accelerated wound healing in a rat skin wound model more effectively within 2 weeks than both the ESF membrane and a commercial dressing (3M™ Tegaderm™). The enhanced wound healing effect of the PESF membranes was further proved by the increase in the content of hydroxyproline (a constituent in collagen) in the wound treated by the PESF membranes. Therefore, the PESF membranes could be used as a promising wound dressing for wound healing and skin regeneration.
Evaluation of bone marrow stem cell response to PLA scaffolds manufactured by 3D printing and coated with polydopamine and type I collagen.
Teixeira Bruna Nunes,Aprile Paola,Mendonça Roberta H,Kelly Daniel J,Thiré Rossana Mara da Silva Moreira
Journal of biomedical materials research. Part B, Applied biomaterials
The majority of synthetic polymers used in 3 D printing are not designed to promote specific cellular interactions and hence possess limited bioactivity. Most of the strategies proposed to overcome this limitation demand multiple and expensive processing steps. This study aimed to evaluate the surface modification of 3D-printed poly(lactic acid) (PLA) scaffolds with polydopamine (PDA) coating as an alternative strategy to enhance their bioactivity and to facilitate the immobilization of type I collagen (COL I) onto the implant surface. Physical and chemical properties of PLA scaffolds coated with PDA, COL I or both were evaluated. The response of porcine bone marrow stem cells (MSCs) to the coatings was also investigated. The PDA layer improved COL immobilization onto the surface of the PLA scaffolds by 92%. The combination of PDA and COL functionalizations provided the best conditions for early-stage (<7 days) cell response. In addition, the PDA plus COL surface facilitated the robust deposition of extracellular matrix in the first 14 days of cell culture. Although the behavior of the MSCs appeared to be similar for both uncoated PLA and PDA plus COL-coated scaffolds by day 21, cells seeded onto PDA plus COL scaffolds produced substantially higher amounts of alkaline phosphatase. These results indicate that the osteoinductivity of 3D-printed PLA scaffolds can be enhanced by PDA and type I collagen coatings. This surface modification of polymeric scaffolds represents a promising strategy for bone tissue engineering. © 2018 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 107B: 37-49, 2019.
Effects of DNase I coating of titanium on bacteria adhesion and biofilm formation.
Ye Jing,Shao Can,Zhang Xu,Guo Xuyun,Gao Ping,Cen Yunzhu,Ma Shiqing,Liu Ying
Materials science & engineering. C, Materials for biological applications
The removal of mature biofilm from the surface of implant has been a formidable challenge in treating implant-associated infection. Prevention of biofilm formation rather than removal of existing biofilm is a more effective approach. Immobilization of biofilm-dispersing enzymes on material surfaces is regarded as one of the most promising strategies. Deoxyribonuclease I (DNase I) can degrade extracellular DNA (eDNA) and then destabilize biofilm. In this study, DNase I was immobilized on a titanium (Ti) surface by using dopamine as an intermediate. The water contact angle, SEM, EDS and XPS confirmed that DNase I was successfully coated to the bare Ti and the final coating was highly hydrophilic. The DNase I coating showed significant effects in preventing Streptococcus mutans (S. mutans) and Staphylococcus aureus (S. aureus) adhesion and biofilm formation over a time span of 24h. The favorable biocompatibility was demonstrated by cell study in vitro. In addition, cell adhesion results suggested that DNase I coating had the potential to facilitate MC3T3-E1 cell attachment. DNase I coating with anti-infection ability and biocompatibility has great potential for increasing success rates of implant applications.
Versatile Polydopamine Platforms: Synthesis and Promising Applications for Surface Modification and Advanced Nanomedicine.
Cheng Wei,Zeng Xiaowei,Chen Hongzhong,Li Zimu,Zeng Wenfeng,Mei Lin,Zhao Yanli
As a mussel-inspired material, polydopamine (PDA), possesses many properties, such as a simple preparation process, good biocompatibility, strong adhesive property, easy functionalization, outstanding photothermal conversion efficiency, and strong quenching effect. PDA has attracted increasingly considerable attention because it provides a simple and versatile approach to functionalize material surfaces for obtaining a variety of multifunctional nanomaterials. In this review, recent significant research developments of PDA including its synthesis and polymerization mechanism, physicochemical properties, different nano/microstructures, and diverse applications are summarized and discussed. For the sections of its applications in surface modification and biomedicine, we mainly highlight the achievements in the past few years (2016-2019). The remaining challenges and future perspectives of PDA-based nanoplatforms are discussed rationally at the end. This timely and overall review should be desirable for a wide range of scientists and facilitate further development of surface coating methods and the production of PDA-based materials.
Layered double hydroxide/poly-dopamine composite coating with surface heparinization on Mg alloys: improved anticorrosion, endothelialization and hemocompatibility.
Li Hua,Peng Feng,Wang Donghui,Qiao Yuqin,Xu Demin,Liu Xuanyong
Magnesium (Mg) and its alloys are promising cardiovascular stent materials due to their favourable physical properties and complete degradation in vivo. However, rapid degradation and poor cytocompatibility hinder their clinical applications. To enhance the corrosion resistance and endothelialization of the AZ31 alloy, a layered double hydroxide (LDH)/poly-dopamine (PDA) composite coating (LDH/PDA) was successfully fabricated. Polarization curves and the electrochemical impedance spectroscopy Nyquist spectrum test proved that the corrosion resistance of the LDH/PDA sample was significantly improved in vitro. The LDH/PDA sample greatly improved the adherence process and the proliferation rate of human umbilical vein endothelial cells (HUVECs). After culturing for 10 days, the number of living HUVECs on the LDH/PDA sample was comparable to that on the Ti sample whereas the cells barely survived on the AZ31 or LDH coating. Furthermore, heparin was immobilized on LDH/PDA via a covalent bond (LDH/PDA/HEP). The corrosion resistance and long-term proliferation of HUVECs after the introduction of heparin were mildly decreased compared with the L/P sample, but were still greatly improved compared with AZ31, the LDH coating and the PDA coating. Furthermore, the LDH/PDA/HEP sample greatly improved the HUVEC migration rate compared with the LDH/PDA sample, and inhibited platelet adhesion which was intense on the LDH/PDA sample. Both LDH/PDA and LDH/PDA/HEP samples had a low hemolysis rate (2.52% and 0.65%, respectively) in vitro and eliminated the adverse biocompatible effects of the direct PDA coating on the AZ31 substrate in vivo. Our results suggest that the LDH/PDA composite coating with further heparinization is a promising method to modify the surface of Mg alloys by significantly improving corrosion resistance, endothelialization and hemocompatibility.
Polydopamine-assisted BMP-2-derived peptides immobilization on biomimetic copolymer scaffold for enhanced bone induction in vitro and in vivo.
Pan Haitao,Zheng Qixin,Guo Xiaodong,Wu Yongchao,Wu Bin
Colloids and surfaces. B, Biointerfaces
In this study, a polydopamine (pDA)-coated PLGA-[Asp-PEG]n scaffold was developed for sustained delivery of bone morphogenetic protein-2 (BMP-2)-derived peptide (designated as P24), and then used to address the hypothesis that P24 peptides delivered from the scaffolds could enhance bone induction in vitro and in vivo. We found pDA coating as compared with physical adsorption could more efficiently mediate the grafting of peptides onto polymer surfaces, and the release of P24 peptides from PLGA-[Asp-PEG]n-pDA-P24 was sustained for about 21 days, while a burst P24 release was observed in initial 4h and almost all peptides were released within 24h in physisorbed PLGA-[Asp-PEG]n-P24 group. In vitro, significantly greater ALP activity and mRNA expressions of osteo-specific markers of rat-derived mesenchymal stem cells (rMSCs) were observed in the sustained delivery system than those in physisorbed PLGA-[Asp-PEG]n-P24 and unmodified PLGA-[Asp-PEG]n groups. In vivo, ectopic bone formation studies showed that the sustained delivery system could induce bone formation to a much greater extent than physisorbed PLGA-[Asp-PEG]n-P24. Meanwhile, there were no evidences of bone formation in non-P24-loaded PLGA-[Asp-PEG]n. It is concluded that PLGA-[Asp-PEG]n-pDA-P24 biomaterial can delivery bioactive P24 peptides in a sustained manner, which can more efficiently promote osteogenic differentiation of rMSCs in vitro and induce ectopic bone formation in vivo, as compared with PLGA-[Asp-PEG]n-P24 delivering P24 in a burst manner. This pDA-coated PLGA-[Asp-PEG]n-pDA-P24 composite promises to be an excellent biomaterial for inducing bone regeneration. Moreover, pDA-mediated catechol functionalization can be an effective, simple technique for developing sustained delivery systems.
Protein immobilization and fluorescence quenching on polydopamine thin films.
Chen Daqun,Zhao Lei,Hu Weihua
Journal of colloid and interface science
Mussel inspired polydopamine (PDA) film has attracted great interest as a versatile functional coating for biomolecule immobilization in various bio-related devices. However, the details regarding the interaction between a protein and PDA film remain unclear. Particularly, there is very limited knowledge regarding the protein immobilization on PDA film, even though it is of essential importance in various fields. The situation is even more complicated if considering the fact that quite a number of approaches (e.g., different oxidizing reagent, buffer pH, grown time, grown media, etc.) have been developed to grow PDA films. In this work, protein attachment on PDA film was systematically investigated by using the real-time and label-free surface plasmon resonance (SPR) technique. The kinetics of protein-PDA interaction was explored and the influence of buffer pH and deposition media on the protein attachment was studied. Fluorescent protein microarray was further printed on PDA-coated glass slides for quantitative investigations and together with SPR data, the interesting fluorescence quenching phenomenon of PDA film was revealed. This work may deepen our understanding on the PDA-protein interaction and offer a valuable guide for efficient protein attachment on PDA film in various bio-related applications.
Mussel-inspired polydopamine-mediated surface modification of freeze-cast poly (ε-caprolactone) scaffolds for bone tissue engineering applications.
Ghorbani Farnaz,Zamanian Ali,Sahranavard Melika
Biomedizinische Technik. Biomedical engineering
There are many methods used to fabricate the scaffolds for tissue regeneration, among which freeze casting has attracted a great deal of attention due to the capability to create a unidirectional structure. In this study, polycaprolactone (PCL) scaffolds were fabricated by freeze-casting technology in order to create porous microstructure with oriented open-pore channels. To induce biomineralization, and to improve hydrophilicity and cell interactions, mussel-inspired polydopamine (PDA) was coated on the surface of the freeze-cast PCL constructs. Then, the synergistic effects of oriented microstructure and deposited layer on efficient reconstruction of injured bone were studied. Microscopic observations demonstrated that, the coated layer did not show any special change in lamellar microstructure of the scaffolds. Water-scaffold interactions were evaluated by contact angle measurements, and they demonstrated strong enhancement in the hydrophilicity of the polymeric scaffolds after PDA coating. Biodegradation ratio and water uptake evaluation confirmed an increase in the measured values after PDA precipitation. The biomineralization of the PDA-coated scaffolds was characterized by field-emission scanning electron microscopy (FE-SEM), energy dispersive X-ray (EDX) and X-ray diffraction (XRD). Obtained results confirmed biomineralization of the constructs after a 28-day immersion in a simulated body fluid (SBF) solution. Mechanical analysis demonstrated higher compressive strength after PDA coating. L929 fibroblast cell viability and attachment illustrated that PDA-coated PCL scaffolds are able to support cell adhesion and proliferation. The increased secretion of alkaline phosphatase (ALP) after culturing osteosarcoma cell lines (MG-63) revealed the initial capability of scaffolds to induce bone regeneration. Therefore, the PDA-coated scaffolds introduce a promising approach for bone tissue engineering application.
Studies on Cell Compatibility, Antibacterial Behavior, and Zeta Potential of Ag-Containing Polydopamine-Coated Bioactive Glass-Ceramic.
Tejido-Rastrilla Rocío,Ferraris Sara,Goldmann Wolfgang H,Grünewald Alina,Detsch Rainer,Baldi Giovanni,Spriano Silvia,Boccaccini Aldo R
Materials (Basel, Switzerland)
Dopamine is a small molecule that mimics the adhesive component (L-DOPA) of marine mussels with a catecholamine structure. Dopamine can spontaneously polymerize to form polydopamine (PDA) in a mild basic environment. PDA binds, in principle, to all types of surfaces and offers a platform for post-modification of surfaces. In this work, a novel Ag-containing polydopamine coating has been developed for the functionalization of bioactive glass-ceramics. In order to study the interactions between the surface of uncoated and coated samples and the environment, we have measured the surface zeta potential. Results confirmed that PDA can interact with the substrate through different chemical groups. A strongly negative surface zeta potential was measured, which is desirable for biocompatibility. The dual function of the material, namely the capability to exhibit bioactive behavior while being antibacterial and not harmful to mammalian cells, was assessed. The biocompatibility of the samples with MG-63 (osteoblast-like) cells was determined, as well as the antibacterial behavior against Gram-positive and Gram-negative bacteria. During cell biology tests, uncoated and PDA-coated samples showed biocompatibility, while cell viability on Ag-containing PDA-coated samples was reduced. On the other hand, antibacterial tests confirmed the strong antimicrobial properties of Ag-containing PDA-coated samples, although tailoring of the silver release will be necessary to modulate the dual effect of PDA and silver.
Stem cell spheroids incorporating fibers coated with adenosine and polydopamine as a modular building blocks for bone tissue engineering.
Ahmad Taufiq,Byun Hayeon,Lee Jinkyu,Madhurakat Perikamana Sajeesh Kumar,Shin Young Min,Kim Eun Mi,Shin Heungsoo
Although stem cell spheroids offer great potential as functional building blocks for bottom-up bone tissue engineering, delivery of bioactive signals remain challenging. Here, we engineered adenosine-ligand-modified fiber fragments to create a 3D cell-instructive microenvironment for bone. Briefly, the Poly(ι-lactic acid) (PLLA) nanofiber sheet was partially degraded into fragmented fibers (FFs) through aminolysis and adenosine was stably incorporated via one-step polydopamine coating. The SEM and XPS analysis demonstrated that polydopamine assisted adenosine coating efficiency was significantly increased, which led to high coating efficiency of adenosine and its significant retention. The engineered fibers were then assembled into stable spheroids with human-adipose-derived stem cells (hADSCs). The adenosine in the spheroids effectively stimulated A2bR (1.768 ± 0.08) signaling, which further significantly induced the expression of osteogenic markers such as Runx2 (3.216 ± 0.25), OPN (4.136 ± 0.14), OCN (10.16 ± 0.34), and OSX (2.27 ± 0.11) with improved mineral deposition (1.375 ± 0.05 μg per spheroid). In contrast, the adipogenic differentiation of hADSCs was significantly suppressed within the engineered spheroids. Transplantation of engineered spheroids strongly induced osteogenic differentiation of hADSCs in ectopic subcutaneous tissue. Finally, the bone regeneration was significantly enhanced by implanting AP-FF group (59.97 ± 18.33%) as compared to P-FF (27.96 ± 11.14) and defect only (7.97 ± 3.76%). We propose that stem cell spheroids impregnated with engineered fibers enabling adenosine delivery could be promising building blocks for a bottom-up approach to create large tissues for regeneration of damaged bone.
Hierarchically Patterned Polydopamine-Containing Membranes for Periodontal Tissue Engineering.
Hasani-Sadrabadi Mohammad Mahdi,Sarrion Patricia,Nakatsuka Nako,Young Thomas D,Taghdiri Nika,Ansari Sahar,Aghaloo Tara,Li Song,Khademhosseini Ali,Weiss Paul S,Moshaverinia Alireza
Periodontitis is a common chronic inflammatory disease that affects tooth-supporting tissues. We engineer a multifunctional periodontal membrane for the guided tissue regeneration of lost periodontal tissues. The major drawback of current periodontal membranes is the lack of tissue regeneration properties. Here, a series of nanofibrous membranes based on poly(ε-caprolactone) with tunable biochemical and biophysical properties were developed for periodontal tissue regeneration. The engineered membranes were surface coated using biomimetic polydopamine to promote the adhesion of therapeutic proteins and cells. We demonstrate successful cellular localization on the surface of the engineered membrane by morphological patterning. Polydopamine accelerates osteogenic differentiation of dental-derived stem cells by promoting hydroxyapatite mineralization. Such multiscale designs can mimic the complex extracellular environment of periodontal tissue and serve as functional tissue constructs for periodontal regeneration. In a periodontal defect model in rats, our engineered periodontal membrane successfully promoted the regeneration of periodontal tissue and bone repair. Altogether, our data demonstrate that our biomimetic membranes have potential as protein/cell delivery platforms for periodontal tissue engineering.
Rapid Deposition of Uniform Polydopamine Coatings on Nanoparticle Surfaces with Controllable Thickness.
Orishchin Nazar,Crane Cameron C,Brownell Matthew,Wang Tengjiao,Jenkins Samuel,Zou Min,Nair Arun,Chen Jingyi
Langmuir : the ACS journal of surfaces and colloids
Polydopamine is a bioinspired, versatile material that can adhere to bulk and nanoscale surfaces made of disparate materials to improve their physical and chemical properties in many applications. The typical methods to coat polydopamine on the nanoparticle substrates usually take several hours to a day. This work successfully applies a dispersion method to form a controllable, uniform coating on a nanoparticle surface within minutes. Using plasmonic Ag nanoparticles as a substrate, the coating thickness can be monitored using a spectroscopic method based on the extinction peak shifts of the Ag nanoparticles. The deposition rate increases with dopamine concentration; however, too much excess dopamine leads to the formation of free dopamine particles. The optimized concentration of dopamine (i.e., ∼6 mM) can be applied to other nanoparticles by normalizing the number of particles to maintain a constant concentration of dopamine per unit surface area (i.e., 1.70 × 10 dopamine/nm). The molecular dynamics simulation reveals that the amount of hydrogen bonding increases with water content, suggesting that sufficient mixing using the dispersion tool facilitates the formation of hydrogen bonding, thus rapidly depositing PDA on the nanoparticle surface. The physical and chemical properties (e.g., pH response and thermal stability) can be tailored by varying the coating thickness due to the changes in the number of hydrogen bonds and the conformation of π-π interactions. This dispersion method provides a facile means to control the PDA coating thickness on nanoparticle surfaces and thus the surface properties of nanoparticles toward various applications.
Polymer-Nanoparticle Interaction as a Design Principle in the Development of a Durable Ultrathin Universal Binary Antibiofilm Coating with Long-Term Activity.
Mei Yan,Yu Kai,Lo Joey C Y,Takeuchi Lily E,Hadjesfandiari Narges,Yazdani-Ahmadabadi Hossein,Brooks Donald E,Lange Dirk,Kizhakkedathu Jayachandran N
Bacterial attachment and biofilm formation pose major challenges to the optimal performance of indwelling devices. Current coating methods have significant deficiencies including the lack of long-term activity, easy of application, and adaptability to diverse materials. Here we describe a coating method that could potentially overcome such limitations and yield an ultrathin coating with long-term antibiofilm activity. We utilized the interaction between polydopamine (PDA) nanoaggregates/nanoparticles and ultrahigh molecular weight (uHMW) hydrophilic polymers to generate stable coatings with broad spectrum antibiofilm activity. We used a short-term bacterial adhesion assay as an initial screening method to identify coating compositions that give superior performance and found that only selected polymers (out of 13 different types) and molecular weights gave promising antifouling activity. Optimization of PDA self-assembly, polymer-PDA interaction, and deposition on the surface using uHMW poly( N,N-dimethylacrylamide) (PDMA) (∼795 kDa) resulted in a stable ultrathin coating (∼19 nm) with excellent antifouling and antibiofilm properties (>4 weeks) against diverse bacteria (∼10 CFU/mL) in shaking and flow conditions. The ultrathin coating is effective on diverse substrates including metals and polymeric substrates. The uHMW PDMA is stabilized in the coating via supramolecular interactions with PDA and generated a surface that is highly enriched with PDMA in aqueous conditions. Based on the surface analyses data, we also propose a mechanism for the stable coating formation. The molecular weight of PDMA is a crucial factor, and only uHMW polymers generate this property. An attractive feature of the coating is that it does not contain any antimicrobial agents and has the potential to prevent biofilm formation for diverse applications both short- and long-term.
Targeted and controlled drug delivery by multifunctional mesoporous silica nanoparticles with internal fluorescent conjugates and external polydopamine and graphene oxide layers.
Tran Anh-Vy,Shim KyuHwan,Vo Thi Thu-Thao,Kook Jeong-Keun,An Seong Soo A,Lee Sang-Wha
This study demonstrated the targeted delivery and controlled release of cisplatin drug molecules from doubly decorated mesoporous silica nanoparticles (MSNs), which were internally grafted with fluorescent conjugates and externally coated with polydopamine (PDA) and graphene oxide (GO) layers. The brush-like internal conjugates conferred fluorescent functionality and high capacity of cisplatin loading into MSNs, as well as contributing to a sustained release of the cisplatin through a porous channel with the assistance of external PDA layer. A consolidated double-layer formed by electrostatic interactions between the GO nanosheet and the PDA layer induced more controlled release kinetics which was well predicted by Higuchi model. In addition, Our MSNs exhibited stimuli (pH, NIR irradiation)-responsive controlled release as a potential chemo-photothermal agent against cancer cells. In a cell test, multifunctional MSNs showed a low toxicity itself, but gave a high cytotoxicity against human epithelial neuroblastoma cells (SH-SY5Y) after loading cisplatin. Notably, GO-wrapped MSNs exhibited very effective drug delivery because GO wrapping enhanced their dispensability in aqueous solution, photothermal heating effect, and efficient endocytosis into cells. Furthermore, monoclonal antibody (anti-human epidermal growth factor receptor)-conjugated MSNs showed a higher specificity, which resulted in more enhanced anticancer effects in vitro. The current study demonstrated a reliable synthesis of multifunctional MSNs, endowed with fluorescent imaging, stimuli-responsive controlled release, higher specificity, and efficient cytotoxicity toward cancer cells. STATEMENT OF SIGNIFICANCE:The current study demonstrated the reliable synthesis of multifunctional mesoporous silica nanoparticles (MSNs) with internal fluorescent conjugates and external polydopamine and graphene oxide (GO) layers. The combination of internal conjugates and external coating layers produced an effective pore closure effect, leading to controlled and sustained release of small drug molecules. Notably, GO wrapping improved the dispensability and cellular uptake of the MSNs, as well as enhanced drug-controlled release. Our multifunctional MSNs revealed very efficient drug delivery effects against human epithelial neuroblastoma cells by demonstrating several strengths: i) fluorescent imaging, ii) sustained and controlled release of small drug molecules, iii) efficient cellular uptake, cytotoxicity and specificity, and v) stimuli (pH, NIR irradiation)-responsive controlled release as a potential chemo-photothermal agent.
Polydopamine mediated assembly of hydroxyapatite nanoparticles and bone morphogenetic protein-2 on magnesium alloys for enhanced corrosion resistance and bone regeneration.
Jiang Yanan,Wang Bi,Jia Zhanrong,Lu Xiong,Fang Liming,Wang Kefeng,Ren Fuzeng
Journal of biomedical materials research. Part A
Magnesium alloys have the great potential to be used as orthopedic implants due to their biodegradability and mechanical resemblance to human cortical bone. However, the rapid degradation in physiological environment with the evolution of hydrogen gas release hinders their clinical applications. In this study, we developed a novel functional and biocompatible coating strategy through polydopamine mediated assembly of hydroxyapatite nanoparticles and growth factor, bone morphogenetic protein-2 (BMP-2), onto the surface of AZ31 Mg alloys. Such functional coating has strong bonding with the substrate and can increase surface hydrophilicity of magnesium alloys. In vitro electrochemical corrosion and hydrogen evolution tests demonstrate that the coating can significantly enhance the corrosion resistance and therefore slow down the degradation of AZ31 Mg alloys. In vitro cell culture reveals that immobilization of HA nanoparticles and BMP-2 can obviously promote cell adhesion and proliferation. Furthermore, in vivo implantation tests indicate that with the synergistic effects of HA nanoparticles and BMP-2, the coating does not cause obvious inflammatory response and can significantly reduce the biodegradation rate of the magnesium alloys and induce the new bone formation adjacent to the implants. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 105A: 2750-2761, 2017.
Enhanced silver loaded antibacterial titanium implant coating with novel hierarchical effect.
Zhang Yanxian,Dong Chaofang,Yang Sefei,Chiu Te-Wei,Wu Junsheng,Xiao Kui,Huang Yunhua,Li Xiaogang
Journal of biomaterials applications
In this study, we present a novel strategy for hierarchical antibacterial implant coating by controlling structural and componential features as regulators of surface bactericidal property. Anodized titanium dioxide nanotubes and self-polymerized polydopamine were both used as preliminary antibacterial agents with a significant positive effect on surface bioactivity. At the same time, the storage capacity of nanotubes and the in situ reduction activity of polydopamine can introduce large amounts of strong attached silver nanoparticles for enhanced stable antibacterial performance. The surface morphology, chemical composition, and hydrophilicity had been thoroughly characterized. The sustained silver release performances were continuously monitored. The successively in vitro inhibition on Staphylococcus aureus growth of titanium dioxide nanotube, polydopamine layer and silver nanoparticles demonstrated the hierarchical antibacterial property of the final silver nanoparticles-incorporated polydopamine-modified titanium dioxide nanotube coating (silver/polydopamine/nanotube). Moreover, the bioactivity investigation indicated the vital role of polydopamine-modified titanium dioxide nanotube coating on preserving healthy osteoblast activity at the implant interface. The unique hierarchical coating for titanium implant may be a promising method to maximize antibacterial capacity and maintain good cellular activity at the same time.
Probing polydopamine adhesion to protein and polymer films: microscopic and spectroscopic evaluation.
Mallinson David,Mullen Alexander B,Lamprou Dimitrios A
Journal of materials science
Polydopamine has been found to be a biocompatible polymer capable of supporting cell growth and attachment, and to have antibacterial and antifouling properties. Together with its ease of manufacture and application, it ought to make an ideal biomaterial and function well as a coating for implants. In this paper, atomic force microscope was used to measure the adhesive forces between polymer-, protein- or polydopamine-coated surfaces and a silicon nitride or polydopamine-functionalised probes. Surfaces were further characterised by contact angle goniometry, and solutions by circular dichroism. Polydopamine was further characterised with infrared spectroscopy and Raman spectroscopy. It was found that polydopamine functionalisation of the atomic force microscope probe significantly reduced adhesion to all tested surfaces. For example, adhesion to mica fell from 0.27 ± 0.7 to 0.05 ± 0.01 nN nm. The results suggest that polydopamine coatings are suitable to be used for a variety of biomedical applications.
A facile method to modify polypropylene membrane by polydopamine coating via inkjet printing technique for superior performance.
Li Renjie,Liu Jinxia,Shi An,Luo Xiaoqian,Lin Jincong,Zheng Ran,Fan Hangxu,Selasie Semekor Vincent,Lin Hongjun
Journal of colloid and interface science
Membrane surface functionalization based on mussel-inspired polydopamine (PDA) deposition for enhancing antifouling ability has attracted considerable attention. However, high cost of dopamine (DA) and long-time of reaction during self-polymerization of DA in aqueous solution remain the major problems impeding its practical application. This study provided a first report on a low-cost and facile membrane modification approach based on inkjet printing of DA and sodium periodate (SP) to rapidly deposit PDA on polypropylene (PP) membrane. Compared with the pristine PP membrane and DA printed PP membrane, the PDA-SP coated PP membrane demonstrated superior hydrophilicity (67.2°), high pure water permeability (2156.8 L·m·h) and antifouling property, due to the improved oxidation degree of PDA. Moreover, the modified membrane possesses good chemical stability in aqueous solution over the wide range of pH 2-9. The inkjet printing integrated oxidant-induced mussel-inspired modification proposed in this study is substrate-independent, and can be applied to various geometries and materials, showing broad application prospects in membrane fabrication.
Tuning the Bandgap of Photo-Sensitive Polydopamine/AgPO/Graphene Oxide Coating for Rapid, Noninvasive Disinfection of Implants.
Xie Xianzhou,Mao Congyang,Liu Xiangmei,Tan Lei,Cui Zhenduo,Yang Xianjin,Zhu Shengli,Li Zhaoyang,Yuan Xubo,Zheng Yufeng,Yeung Kelvin Wai Kwok,Chu Paul K,Wu Shuilin
ACS central science
Bacterial infection and associated complications are threats to human health especially when biofilms form on biomedical devices and artificial implants. Herein, a hybrid polydopamine (PDA)/AgPO/graphene oxide (GO) coating is designed and constructed to achieve rapid bacteria killing and eliminate biofilms in situ. By varying the amount of GO in the hybrid coating, the bandgap can be tuned from 2.52 to 2.0 eV so that irradiation with 660 nm visible light produces bacteria-killing effects synergistically in concert with reactive oxygen species (ROS). GO regulates the release rate of Ag to minimize the cytotoxicity while maintaining high antimicrobial activity, and a smaller particle size enhances the yield of ROS. After irradiation with 660 nm visible light for 15 min, the antimicrobial rates of the PDA/AgPO/GO hybrid coating against and are 99.53% and 99.66%, respectively. In addition, this hybrid coating can maintain a repeatable and sustained antibacterial efficacy. The released Ag and photocatalytic AgPO produce synergistic antimicrobial effects in which the ROS increases the permeability of the bacterial membranes to increase the probability of Ag to enter the cells to kill them together with ROS synergistically.
Icariin immobilized electrospinning poly(l-lactide) fibrous membranes via polydopamine adhesive coating with enhanced cytocompatibility and osteogenic activity.
Liu Hua,Li Wenling,Luo Binghong,Chen Xuexing,Wen Wei,Zhou Changren
Materials science & engineering. C, Materials for biological applications
In this study, icariin (ICA), one of the main active ingredients of Herba Epimedii for osteogenesis, was applied to functionalize electrospinning poly(l-lactide) (PLLA) fibrous membrane via an intermediate layer of polydopamine (PDA) to obtain enhanced cytocompatibility and osteogenic activity. For this purpose, an array of PDA-coated PLLA fibrous membranes (PLLA-0.5PDA, PLLA-1PDA, PLLA-2PDA, PLLA-5PDA) and ICA-modified PLLA-2PDA fibrous membranes (PLLA-2PDA-10ICA, PLLA-2PDA-20ICA, PLLA-2PDA-40ICA) were successively prepared. Successful modification of PDA and ICA onto PLLA fibrous membranes was verified by field emission scanning electron microscope (FESEM), thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS). Besides, the hydrophilicity as well as tensile properties of PLLA fibrous membrane were improved after surface modified with PDA and ICA. In vitro cells culture experiments revealed that the adhesion, proliferation and osteogenic differentiation of MC3T3-E1 cells on the PLLA fibrous membrane were significantly improved by successively immobilized with PDA and ICA. Moreover, the concentration of ICA immobilized on the fibrous membranes has the complicated effects on the MC3T3-E1 cells behavior. The PLLA-2PDA-ICA fibrous membranes with low ICA concentration promoted the cell adhesion and proliferation, but on the contrary, those with high ICA concentration were more beneficial to the enhancement in ALP activity and calcium deposition.
Graded functionalization of biomaterial surfaces using mussel-inspired adhesive coating of polydopamine.
Perikamana Sajeesh Kumar Madhurakkat,Shin Young Min,Lee Jin Kyu,Lee Yu Bin,Heo Yunhoe,Ahmad Taufiq,Park So Yeon,Shin Jisoo,Park Kyung Min,Jung Hyun Suk,Cho Seung-Woo,Shin Heungsoo
Colloids and surfaces. B, Biointerfaces
Biomaterials with graded functionality have various applications in cell and tissue engineering. In this study, by controlling oxidative polymerization of dopamine, we demonstrated universal techniques for generating chemical gradients on various materials with adaptability for secondary molecule immobilization. Diffusion-controlled oxygen supply was successfully exploited for coating of polydopamine (PD) in a gradient manner on different materials, regardless of their surface chemistry, which resulted in gradient in hydrophilicity and surface roughness. The PD gradient controlled graded adhesion and spreading of human mesenchymal stem cells (hMSCs) and endothelial cells. Furthermore, the PD gradient on these surfaces served as a template to allow for graded immobilization of different secondary biomolecules such as cell adhesive arginine-glycine-aspartate (RGD) peptides and siRNA lipidoid nanoparticles (sLNP) complex, for site-specific adhesion of human mesenchymal stem cells, and silencing of green fluorescent protein (GFP) expression on GFP-HeLa cells, respectively. In addition, the same approach was adapted for generation of nanofibers with surface in graded biomineralization under simulated body fluid (SBF). Collectively, oxygen-dependent generation of PD gradient on biomaterial substrates can serve as a simple and versatile platform that can be used for various applications realizing in vivo tissue regeneration and in vitro high-throughput screening of biomaterials.
Gelatin Hydrogel Combined with Polydopamine Coating to Enhance Tissue Integration of Medical Implants.
Dinh Thanh N,Hou Shujie,Park Shiwha,Shalek Benjamin A,Jeong Kyung Jae
ACS biomaterials science & engineering
Soft tissue integration of medical implants is important to prevent bacterial infection and implant failure. A bioadhesive that forms firm binding between the implant and the surrounding tissue and facilitates the wound-healing process will be a great tool to establish the desired tissue-implant integration. In this project, we introduce a novel method that can be used to enhance integration between any implant material and any tissue using an enzyme-crosslinked gelatin hydrogel combined with polydopamine (PDA) coating. PDA coating was shown to enhance the binding between the gelatin hydrogel and three model implant materials - aluminum, poly(methyl methacrylate) (PMMA) and titanium. When combined with the gelatin hydrogel, pig cornea tissue adhered more strongly to the PDA coated surfaces than to the uncoated surfaces. The enzyme-crosslinked gelatin hydrogel was non-cytotoxic to human dermal fibroblasts and it also allowed the cells to adhere and proliferate. Altogether, the results indicate that the combination of PDA coating with gelatin hydrogel can be used to enhance the integration of various medical implants.
Material-Independent Surface Chemistry beyond Polydopamine Coating.
Lee Haesung A,Ma Yanfei,Zhou Feng,Hong Seonki,Lee Haeshin
Accounts of chemical research
Various methods have been developed in surface chemistry to control interface properties of a solid material. A selection rule among surface chemistries is compatibility between a surface functionalization tool and a target material. For example, alkanethiol deposition on noble metal surfaces, widely known as the formation of a self-assembled monolayer (SAM), cannot be performed on oxide material surfaces. One must choose organosilane molecules to functionalize oxide surfaces. Thus, the surface chemistry strictly depends on the properties of the surface. Polydopamine coating is now generally accepted as the first toolbox for functionalization of virtually any material surface. Layer-by-layer (LbL) assembly is a widely used method to modify properties of versatile surfaces, including organic materials, metal oxides, and noble metals, along with polydopamine coating. On flat solid substrates, the two chemistries of polydopamine coating and LbL assembly provide similar levels of surface modifications. However, there are additional distinct features in polydopamine. First, polydopamine coating is effective for two- or three-dimensional porous materials such as metal-organic frameworks (MOFs), synthetic polyolefin membranes, and others because small-sized dopamine (MW = 153.18 u) and its oxidized oligomers are readily attached onto narrow-spaced surfaces without exhibiting steric hindrance. In contrast, polymers used in LbL assembly are slow in diffusion because of steric hindrance due to their high molecular weight. Second, it is applicable to structurally nonflat surfaces showing special wettability such as superhydrophobicity or superoleophobicity. Third, a nonconducting, insulating polydopamine layer can be converted to be a conducting layer by pyrolysis. The product after pyrolysis is a N-doped graphene-like material that is useful for graphene or carbon nanotube-containing composites. Fourth, it is a suitable method for engineering the surface properties of various composite materials. The surface properties of participating components in composite materials can be unified by polydopamine coating with a simple one-step process. Fifth, a polydopamine layer exhibits intrinsic chemical reactivity by the presence of catecholquinone moieties and catechol radical species on surfaces. Nucleophiles such as amine and thiolate spontaneously react with the functionalized layer. Applications of polydopamine coating are exponentially growing and include cell culture/patterning, microfluidics, antimicrobial surfaces, tissue engineering, drug delivery systems, photothermal therapy, immobilization of photocatalysts, Li-ion battery membranes, Li-sulfur battery cathode materials, oil/water separation, water detoxification, organocatalysts, membrane separation technologies, carbonization, and others. In this Account, we describe various polydopamine coating methods and then introduce a number of chemical derivatives of dopamine that will open further development of material-independent surface chemistry.
Bioinspired and Biomimetic AgNPs/Gentamicin-Embedded Silk Fibroin Coatings for Robust Antibacterial and Osteogenetic Applications.
Zhou Wenhao,Jia Zhaojun,Xiong Pan,Yan Jianglong,Li Yangyang,Li Ming,Cheng Yan,Zheng Yufeng
ACS applied materials & interfaces
With the progressively increasing demand for orthopedic Ti implants, the balance between two primary complications restricting implant applications is needed to be solved: the lack of bone tissue integration and biomedical device-associated infections (BAI), where emergence of multiresistance bacteria make it worse. Notably, a combination of silver nanoparticles (AgNPs) and a kind of antibiotic can synergistically inhibit bacterial growth, where a low concentration of AgNPs has been confirmed to promote the proliferation and osteogenesis of osteoblasts. In this work, we built AgNPs/gentamicin (Gen)-embedded silk fibroin (SF)-based biomimetic coatings on orthopedic titanium by a facile dipping-drying circular process and with the assistance of polydopamine (PD). Ag was reduced to AgNPs by SF under ultraviolet (UV) irradiation, and then they were detected by transmission electron microscope (TEM) images and UV-visible (UV-vis) analyses. Intriguingly, the addition of Gen highly improved the reduction efficiency of Ag. The antibacterial efficiency of SF-based coatings was examined by challenging them with pathogenic Staphylococcus aureus (S. aureus) bacteria which produced biofilms, and consequently, we found that low concentration loading, durable release of Ag (28 days), and 10-fold improvement of antibacterial efficiency were achieved for our novel AgNPs- and Gen-embeded silk fibroin coatings. In bacteria and a cells cocultured system, AgNPs/Gen-embedded coatings strongly inhibited adhesion and proliferation of S. aureus, simultaneously improving cell adhesion and growth. To investigate cytocompatibility and osteogenic potential, different coatings were cultured with MC3T3 cells; AgNPs/Gen-embedded coatings showed generally acceptable biocompatibility (cell adhesion, proliferation, and viability) and accelerated osteoblast maturation (alkaline phosphatase production, matrix secretion, and calcification). Expectantly, this novel biofunctional coating will have promising applications in orthopedic and dental titanium implants thanks to its excellently antibacterial, biocompatible, and osteogenic activities.
Triple-functional polyetheretherketone surface with enhanced bacteriostasis and anti-inflammatory and osseointegrative properties for implant application.
Xu Xiao,Li Yongliang,Wang Lixin,Li Yan,Pan Jijia,Fu Xiaoming,Luo Zuyuan,Sui Yi,Zhang Siqi,Wang Liang,Ni Yaofeng,Zhang Lei,Wei Shicheng
Polyetheretherketone (PEEK) is considered a potential orthopedic/dental material because of its excellent mechanical and chemical properties (e.g., similar elastic modulus to that of human bone). However, the poor bacteriostasis and anti-inflammatory and osseointegrative properties of bioinert PEEK impede its clinical application. We previously developed a facile and versatile surface modification method using dexamethasone plus minocycline-loaded liposomes (Dex/Mino liposomes) bonded by a mussel-inspired polydopamine coating, which effectively modulated cell inflammatory response and discouraged bacterial colonization in vitro. Herein, we report the application of this multifunctional surface modification method to improve bioinert PEEK, aimed at further studying the in vitro osteogenesis and in vivo properties of Dex/Mino liposome-modified PEEK to prevent bacterial contamination, attenuate the inflammatory response, and enhance ossification for physiologic osseointegration. Our study established that the Dex/Mino liposome-modified PEEK surface presented favorable stability and cytocompatibility. Compared with bare PEEK, improved osteogenic differentiation of human mesenchymal stem cells under both osteoinductive and osteoconductive conditions was found on the functionalized surface due to the liposomal Dex releasing. In vivo bacteriostasis assay confirmed that Mino released from the functionalized surface provided an effective antibacterial effect. Moreover, the subcutaneous foreign body reaction and beagle femur implantation models corroborated the enhanced anti-inflammatory and osteointegrative properties of the functionalized PEEK. Our findings indicate that the developed Dex/Mino liposome-modified PEEK with enhanced antibacterial, anti-inflammatory, and osseointegrative capacity has great potential as an orthopedic/dental implant material for clinical application.
Lithium doped silica nanospheres/poly(dopamine) composite coating on polyetheretherketone to stimulate cell responses, improve bone formation and osseointegration.
Zhang Jue,Cai Liang,Wang Tinglan,Tang Songchao,Li Quan,Tang Tingting,Wei Shicheng,Qian Jun,Wei Jie,Su Jiacan
Nanomedicine : nanotechnology, biology, and medicine
Osseointegration is crucial for early fixation as well as long-term success of orthopedic implants. Bioactive composite containing lithium doping silica nanospheres (LSNs) and poly(dopamine) (PDA) were coated on polyetheretherketone (PK) surface (LPPK), and effects of the LSNs/PDA composite (LPC) coating on the biological properties of LPPK were assessed both in vitro and in vivo. Results showed that LPPK with improved bioactivity remarkably promoted apatite mineralization in simulated body fluid (SBF) compared with PDA coated on PK (PPK) and PK. Moreover, the LPPK remarkably stimulated rat bone marrow stromal cells (rBMSCs) responses compared with PPK and PK. Furthermore, the LPPK significantly promoted bone tissues responses in vivo compared with PPK and PK. It could be suggested that the improvements of cells and bone tissues responses were attributed to the surface characteristics of the bioactive LPC coating on LPPK. The LPPK would be a great candidate for orthopedic and dental applications.
Effect of mussel adhesive protein coating on osteogenesis in vitro and osteointegration in vivo to alkali-treated titanium with nanonetwork structures.
Yin Derong,Komasa Satoshi,Yoshimine Shigeki,Sekino Tohru,Okazaki Joji
International journal of nanomedicine
On the basis of reasonable superposition of various surface treatment methods, alkali-treated titanium with nanonetwork structures (TNS) was coated with mussel adhesive protein (MAP) and named TNS-MAP. The aims were to optimize the biological properties of TNS, endue it with new properties, and enhance its utility in clinical dental applications. TNS disks were coated with MAP and the product surface was characterized. Its osteogenic properties were determined by evaluating its effects on cell adhesion, cell proliferation, the expression of osteogenesis-related genes, and in vivo experiments. The treated materials showed excellent hydrophilicity, good surface roughness, and advantages of both TNS and MAP. TNS-MAP significantly promoted initial cell attachment especially after 15 mins and 30 mins. At every time point, cell adhesion and proliferation, the detection rate of osteogenesis-related markers in the extracellular matrix, and the expression of osteogenesis-related genes were markedly superior on TNS-MAP than the control. The in vivo experiments revealed that TNS-MAP promoted new bone growth around the implants and the bone-implant interface. We verified through in vitro and in vivo experiments that we successfully created an effective TNS-MAP composite implant with excellent biocompatibility and advantages of both its TNS and MAP parent materials. Therefore, the new biocomposite implant material TNS-MAP may potentially serve in practical dentistry and orthopedics.
Polydopamine coating promotes early osteogenesis in 3D printing porous Ti6Al4V scaffolds.
Li Lan,Li Yixuan,Yang Longfei,Yu Fei,Zhang Kaijia,Jin Jing,Shi Jianping,Zhu Liya,Liang Huixin,Wang Xingsong,Jiang Qing
Annals of translational medicine
Background:Titanium implants are widely used in orthopedic and dental for more than 30 years. Its stable physicochemical properties and mechanical strength are indeed appropriate for implantation. However, the Bioinertia oxidized layer and higher elastic modulus often lead to the early implantation failure. Methods:In this study, we proposed a simple design of porous structure to minimize the disparity between scaffold and natural bone tissue, and introduced a one-step reaction to form a polydopamine (PDA) layer on the surface of titanium for the purpose of improving osteogenesis as well. The porous scaffolds with pore size of 400 µm and porosity of 44.66% were made by additive manufacturing. The cell behavior was tested by seeding MC3T3-E1 cells on Ti6Al4V films for 15 days. The biomechanical properties were then analyzed by finite element (FE) method and the osteogenesis effect was accordingly evaluated by implanting the scaffolds for 5 weeks in rabbits. Results:According to the achieved results, it was revealed that the immersion for 40 min with dopamine could significantly improve the cell adhesion. The proposed method for design of porous structure can avoid the stress shielding effect and bone growth inside the PDA coating scaffolds, which were observed at the early stage of bone healing process. Conclusions:It can be concluded that the proposed PDA coating method is effective in promoting early osteogenesis, as well as being easy to operate, and can be helpful in the future clinical application of titanium implants.
Polydopamine-assisted chlorhexidine immobilization on medical grade stainless steel 316L: Apatite formation and in vitro osteoblastic evaluation.
Mohd Daud Nurizzati,Hussein Al-Ashwal Rania,Abdul Kadir Mohammed Rafiq,Saidin Syafiqah
Annals of anatomy = Anatomischer Anzeiger : official organ of the Anatomische Gesellschaft
Immobilization of chlorhexidine (CHX) on stainless steel 316L (SS316L), assisted by a polydopamine film as an intermediate layer is projected as an approach in combating infection while aiding bone regeneration for coating development on orthopedic and dental implants. This study aimed to investigate the ability of CHX coating to promote apatite layer, osteoblast cells viability, adhesion, osteogenic differentiation and mineralization. Stainless steel 316L disks were pre-treated, grafted with a polydopamine film and immobilized with different concentrations of CHX (10-30mM). The apatite layer formation was determined through an in vitro simulated body fluid (SBF) test by ATR-FTIR and SEM-EDX analyses. The osteoblastic evaluations including cells viability, cells adhesion, osteogenic differentiation and mineralization were assessed with human fetal osteoblast cells through MTT assay, morphology evaluation under FESEM, ALP enzyme activity and Alizarin Red S assay. The apatite layer was successfully formed on the CHX coated disks, demonstrating potential excellent bioactivity property. The CHX coatings were biocompatible with the osteoblast cells at low CHX concentration (<20mM) with good adhesion on the metal surfaces. The increment of ALP activity and calcium deposition testified that the CHX coated disks able to support osteoblastic maturation and mineralization. These capabilities give a promising value to the CHX coating to be implied in bone regeneration area.
Enhanced antibacterial activity of titanium by surface modification with polydopamine and silver for dental implant application.
Choi Soo-Hyoen,Jang Yong-Seok,Jang Jong-Hwa,Bae Tae-Sung,Lee Sook-Jeong,Lee Min-Ho
Journal of applied biomaterials & functional materials
BACKGROUND:Biofilm formation and microbial colonization on the surface of implant devices may cause dental caries and peri-implantitis. Therefore, various surface treatments have been developed to improve the antibacterial activity of titanium implant. METHODS:Silver-loaded polydopamine coating was formed by immersing pure titanium in dopamine hydrochloride/HCl buffer solution for 24 h in 50 mL silver nitrate solutions with different concentrations for 30 min. Microbial growth inhibition and microbial growth curve analyses for bacterial solutions of and incubated with the specimens were respectively conducted by counting the numbers of colonies on agar solid medium and by measuring absorbance using enzyme-linked immunosorbent assay reader. RESULTS:Silver nanoparticles were uniformly distributed over the whole surface of the polydopamine and silver-coated titanium specimens. The numbers of microbial colonies for both bacteria cultured with surface-modified titanium were significantly lower than those cultured with uncoated titanium. When and were cultured with surface-modified titanium, the lag phase of the growth curves for both bacteria was continually maintained, whereas the lag phase for and changed to exponential phase after 9 and 15 h, respectively, when both bacteria were cultured with uncoated titanium. CONCLUSION:It was confirmed that the coating of polydopamine and silver on the surface of titanium effectively retards the microbial growth, which can cause the formation of biofilm and pathogenesis of gum disease in the mouth.
PolyDOPA Mussel-Inspired Coating as a Means for Hydroxyapatite Entrapment on Polytetrafluoroethylene Surface for Application in Periodontal Diseases.
Nardo Tiziana,Chiono Valeria,Ciardelli Gianluca,Tabrizian Maryam
Inert polytetrafluoroethylene (PTFE) membranes for periodontal regeneration suffer from weak osteoconductive properties. In this work, a strategy for hydroxyapatite (HAp) coating on PTFE films through an adhesive layer of self-polymerized 3,4-dihydroxy-DL-phenylalanine (polyDOPA) was developed to improve surface properties. Physico-chemical and morphological analysis demonstrated the deposition of polyDOPA and HAp, with an increase in surface roughness and wettability. A discontinuous coating was present after 14 days in PBS and MC3T3-E1 cells proliferation and adhesion were improved. Results confirmed the potential application of polyDOPA/HAp-coated films for periodontal disease treatments.
Inhibition of Cariogenic Plaque Formation on Root Surface with Polydopamine-Induced-Polyethylene Glycol Coating.
Mei May Lei,Li Quan-Li,Chu Chun Hung
Materials (Basel, Switzerland)
Root caries prevention has been a challenge for clinicians due to its special anatomical location, which favors the accumulation of dental plaque. Researchers are looking for anti-biofouling material to inhibit bacterial growth on exposed root surfaces. This study aimed to develop polydopamine-induced-polyethylene glycol (PEG) and to study its anti-biofouling effect against a multi-species cariogenic biofilm on the root dentine surface. Hydroxyapatite disks and human dentine blocks were divided into four groups for experiments. They received polydopamine-induced-PEG, PEG, polydopamine, or water application. Contact angle, quartz crystal microbalance, and Fourier transform infrared spectroscopy were used to study the wetting property, surface affinity, and an infrared spectrum; the results indicated that PEG was induced by polydopamine onto a hydroxyapatite disk. Salivary mucin absorption on hydroxyapatite disks with polydopamine-induced-PEG was confirmed using spectrophotometry. The growth of a multi-species cariogenic biofilm on dentine blocks with polydopamine-induced-PEG was assessed and monitored by colony-forming units, confocal laser scanning microscopy, and scanning electron microscopy. The results showed that dentine with polydopamine-induced-PEG had fewer bacteria than other groups. In conclusion, a novel polydopamine-induced-PEG coating was developed. Its anti-biofouling effect inhibited salivary mucin absorption and cariogenic biofilm formation on dentine surface and thus may be used for the prevention of root dentine caries.
Dopamine Modified Organic-Inorganic Hybrid Coating for Antimicrobial and Osteogenesis.
Li Man,Liu Xiangmei,Xu Ziqiang,Yeung K W K,Wu Shuilin
ACS applied materials & interfaces
A hybrid coating composed of hydroxyapatite (HA), Ag nanoparticles (NPs), and chitosan (CS) was successfully prepared on a Ti substrate by a layer-by-layer assembly process. A polydopamine-assisted (PDA-assisted) coating showed a good bond with HA. Ag NPs were uniformly distributed into the hybrid coating through a solution method and ultraviolet light reduction. A CS nanofilm was deposited via spin-coating to control the release of Ag from the hybrid coating. The results disclosed that the 3-layer CS coating could efficiently control the release of Ag from the hybrid coating via the Fickian diffusion mechanism and that the PDA/HA/Ag/CS-1 coating exhibited antibacterial ratios of 63.0% and 51.8% against E. coli and S. aureus, respectively. Furthermore, the normal structure of E. coli was obviously destroyed by two types of Ag doped coatings. The cell viability assay showed that CS effectively reduced the cytotoxicity of the hybrid coating after a 7 day incubation. The hybrid coating presented high ALP activities at days 3 and 14. The results reveal that hybrid coatings can endow Ti implants with good antibacterial capability as well as cell viability and osteogenic activity.
BMP-2 immobilized PLGA/hydroxyapatite fibrous scaffold via polydopamine stimulates osteoblast growth.
Zhao Xingyu,Han Yu,Li Jiawei,Cai Bo,Gao Hang,Feng Wei,Li Shuqiang,Liu Jianguo,Li Dongsong
Materials science & engineering. C, Materials for biological applications
Combining biomaterials scaffolds with bone morphogenetic protein-2 (BMP-2) is currently used to promote the regeneration of bone tissue. However, the traditional strategies used to add BMP-2 into the polymer scaffolds directly suffer from limitations that can result in lower growth factor loading and damage the bioactivity of growth factors. In this study, we report the fabrication of poly(lactide-co-glycolide)/hydroxyapatite (PLGA/HA) composite fibrous scaffolds via melt-spinning method to mimic native extracellular matrix (ECM). In order to effectively immobilize BMP-2 on PLGA/HA composite fibrous scaffolds, the surface of the scaffold was modified with polydopamine (PDA) (PDA-PLGA/HA). PDA was chosen as an adhesive polymeric bridge-layer between PLGA/HA fibrous scaffolds and BMP-2. Analysis of the scaffold using scanning electron microscopy, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscope revealed that the PDA coating was attached to the scaffold surface. Moreover, analysis of the scaffold using water contact angle demonstrated an increased hydrophilicity via PDA modification. Furthermore, the PDA coating effectively immobilized BMP-2 on the PDA-PLGA/HA fibrous scaffold and a sustained release profile of BMP-2 was achieved in the BMP-2-immobilized PLGA/HA fibrous scaffold. In vitro experiments showed that BMP-2-immobilized PLGA/HA fibrous scaffold significantly promoted the attachment and proliferation of MC3T3-E1 cells. More importantly, the ALP activity, mRNA expression of osteosis-related genes and calcium deposition in MC3T3-E1 cells cultured on BMP-2-immobilized PLGA/HA fibrous scaffold were significantly increased. These results collectively demonstrate that the BMP-2-immobilized PLGA/HA fibrous scaffold is a promising candidate for bone regeneration.
Fabrication of dopamine modified polylactide-poly(ethylene glycol) scaffolds with adjustable properties.
Shen Jiali,Shi Dongjian,Shi Chang,Li Xiaojie,Chen Mingqing
Journal of biomaterials science. Polymer edition
Bio-based polymers have been widely used to be as scaffolds for repairing the bone defects. However, the polymer scaffolds are generally lack of bioactivity and cell recognition site. Seeking effective ways to improve the bioactivity and interaction between materials and tissue or cells is clinically important for long-term performance of bone repair materials. In this work, polylactide-b-poly(ethylene glycol)-b-polylactide (PLA-PEG-PLA, PLEL) tri-block copolymers were firstly synthesized by ring-opening polymerization of lactide using PEG with various molecular weights. Inspired by excellent adhesion of dopamine (DA), a facile and effective method was developed to fabricate polydopamine (PDA) and polydopamine/nano-hydroxyapatite (PDA/n-HA) modified PLEL scaffolds by deposition of PDA and PDA/n-HA coating. The surface structure, degradation rates and mineralization of the modified PLEL scaffolds were investigated, and obviously improved after immobilization of PDA and PDA/n-HA coatings. Moreover, the biocompatible results showed a significant increase in cells viability and adhesion. Therefore, the surface modification with PDA and PDA/n-HA could not only adjust the properties of scaffolds, but also reinforce the interfacial adhesion between the PLEL and cells.
Immobilisation of hydroxyapatite-collagen on polydopamine grafted stainless steel 316L: Coating adhesion and in vitro cells evaluation.
Tapsir Zafirah,Jamaludin Farah H,Pingguan-Murphy Belinda,Saidin Syafiqah
Journal of biomaterials applications
The utilisation of hydroxyapatite and collagen as bioactive coating materials could enhance cells attachment, proliferation and osseointegration. However, most methods to form crystal hydroxyapatite coating do not allow the incorporation of polymer/organic compound due to production phase of high sintering temperature. In this study, a polydopamine film was used as an intermediate layer to immobilise hydroxyapatite-collagen without the introduction of high sintering temperature. The surface roughness, coating adhesion, bioactivity and osteoblast attachment on the hydroxyapatite-collagen coating were assessed as these properties remains unknown on the polydopamine grafted film. The coating was developed by grafting stainless steel 316L disks with a polydopamine film. Collagen type I fibres were then immobilised on the grafted film, followed by the biomineralisation of hydroxyapatite. The surface roughness and coating adhesion analyses were later performed by using AFM instrument. An Alamar Blue assay was used to determine the cytotoxicity of the coating, while an alkaline phosphatase activity test was conducted to evaluate the osteogenic differentiation of human fetal osteoblasts on the coating. Finally, the morphology of cells attachment on the coating was visualised under FESEM. The highest RMS roughness and coating adhesion were observed on the hydroxyapatite-collagen coating (hydroxyapatite-coll-dopa). The hydroxyapatite-coll-dopa coating was non-toxic to the osteoblast cells with greater cells proliferation, greater level of alkaline phosphate production and more cells attachment. These results indicate that the immobilisation of hydroxyapatite and collagen using an intermediate polydopamine is identical to enhance coating adhesion, osteoblast cells attachment, proliferation and differentiation, and thus could be implemented as a coating material on orthopaedic and dental implants.
Dopamine self-polymerized along with hydroxyapatite onto the preactivated titanium percutaneous implants surface to promote human gingival fibroblast behavior and antimicrobial activity for biological sealing.
Yang Minggang,Jiang Peipei,Ge Yang,Lan Fang,Zhou Xuedong,He Jing,Wu Yao
Journal of biomaterials applications
The clinical success of dental implants requires not only the optimum osseointegration but also the integration of implant surface with soft tissues to form biological sealing. In this study, alkali-heat treatment was applied to modify the pure titanium surface constructing a unique micro-and nano-structure. Then, poly(dopamine), along and with the additional incorporation of hydroxyapatite and carboxymethyl chitosan have been successfully infiltrated into the preactivated Ti surface during dopamine self-polymerization proceeding. Here, the effects of poly(dopamine)-modified surface coating on the biological behaviors of human gingival fibroblasts (HGFs) and oral pathogens have been systematically studied, which was critical for the early peri-implant soft tissue integration. The results showed that the poly(dopamine)-modified alkali-heat-titanium surface was a superior substrate for human gingival fibroblast adhesion, spread and proliferation. Moreover, further enhancements on cytoskeleton organization, collagen secretion and fibronectin adsorption were generally observed through the additional incorporation of hydroxyapatite. The addition of carboxymethyl chitosan exerted a positive modulation effect on antibacterial activity. Overall, our study demonstrated that combined superior soft tissue integration and antibacterial activity can be achieved by using poly(dopamine)-modified titanium implant, which has great potential in the optimal design of dental implant.
Incorporating catechol into electroactive polypyrrole nanowires on titanium to promote hydroxyapatite formation.
Wang Zhengao,Zeng Jinquan,Tan Guoxin,Liao Jingwen,Zhou Lei,Chen Junqi,Yu Peng,Wang Qiyou,Ning Chengyun
To improve the osteointegration property of biomedical titanium, nano-architectured electroactive coating was synthesized through the electrochemical polymerization of dopamine and pyrrole. The highly binding affinity of Ca to the catechol moiety of doped dopamine enabled efficient interaction between polypyrrole/polydopamine nanowires and mineral ions. The results indicate that the PPy/PDA nanowires preserved its efficient electro-activity and accelerated the hydroxyapatite deposition in a simulated body fluid. The PPy/PDA nanowires coating could be applied to promote the osteointegration of titanium implant.
Improving Hydrophilicity and Inducing Bone-Like Apatite Formation on PPBES by Polydopamine Coating for Biomedical Application.
Liu Chengde,Li Yizheng,Wang Jinyan,Liu Cheng,Liu Wentao,Jian Xigao
Molecules (Basel, Switzerland)
Copoly(phthalazinone biphenyl ether sulfone) (PPBES) as a commercially available polyarylether is a promising orthopaedic implant material because its mechanical properties are similar to bone. However, the bioinert surface of polyarylether causes some clinical problems after implantation, which limits its application as an implant material. In this study, the surface of PPBES was modified by a biomineralization method of polydopamine-assisted hydroxyapatite formation (pHAF) to enhance its cytocompatibility. Polydopamine (PDA) coating, inspired by the adhesion mechanism of mussels, can readily endow PPBES with high hydrophilicity and the ability to integrate via the bone-like apatite coating. PPBES and PDA-coated PPBES were evaluated by scanning electronic microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and contact angle measurement. The water contact angles were reduced significantly after coating with PDA. PDA was successfully synthesized on PPBES and more PDA was obtained by increasing the temperature. Bone-like apatite on PPBES (apatite-coated PPBES) was confirmed by SEM and transmission electron microscopy (TEM). The cytotoxicity of pristine PPBES and apatite-coated PPBES were characterized by culturing of NIH-3T3 cells. Bone-like apatite synthesized by pHAF could further enhance cytocompatibility in vitro. This study provides a promising alternative for biofunctionalized PPBES with improved cytocompatibility for bone implant application.
Peptide LL-37 coating on micro-structured titanium implants to facilitate bone formation in vivo via mesenchymal stem cell recruitment.
He Ye,Mu Caiyun,Shen Xinkun,Yuan Zhang,Liu Ju,Chen Weizhen,Lin Chuanchuan,Tao Bailong,Liu Bin,Cai Kaiyong
Titanium (Ti) and Ti-alloys were widely used in clinic orthopedics, however, the insufficient bone formation surrounding Ti-based implants still limited their biological performances. Surface modification of Ti substrates is essential to improve their interactions with bone-forming cells and bone tissue. In this study, we modified Ti substrates by coating peptide LL-37 onto micro-structured Ti substrates and aimed to (i) induce mesenchymal stem cells (MSCs) migration both in vitro and in vivo, (ii) facilitate osteogenic differentiation of MSCs and new bone formation. The surface micro-structured Ti substrates with hydroxyapatite deposition were fabricated by a two-step method including micro-arc oxidation (MAO) and hydrothermal treatment. LL-37 was loaded on micro-structured Ti substrates with the assistance of polydopamine coating. We confirmed that surface-modified Ti substrates benefited viability, adhesion, migration and osteogenic differentiation of MSCs in vitro. In a femur-defect rat model, the surface-modified Ti implants effectively induced CD29/CD90 positive cells migration in one week after implantation. According to the results of H&E, Masson's trichrome staining and immunohistochemical staining of OCN, OPN and collagen I, the targeted Ti implants exhibited significant new bone formation after implantation for 4 weeks. These results indicate that the surface modification of Ti samples facilitated bone formation through MSCs recruitment. STATEMENT OF SIGNIFICANCE: The inherent surface bioinertness of titanium (Ti) and Ti-alloys still limits their biological performances in clinical applications. Recently, the strategy of mesenchymal stem cells (MSCs) recruitment has been proposed to improve the osteointegration of bone implants. Herein, we reports the surface modification of Ti implants from the point of MSCs recruitment. Peptide LL-37 was coated on micro-structured Ti substrates to (i) recruit MSCs, (ii) regulate bio-physiological performance of MSCs, and (iii) facilitate bone formation in vivo. Our results improve the understanding of the interaction between Ti implants and MSCs, and provide a promising strategy of MSCs recruitment in the design of bone repair related biomaterials.
Long-Term Prevention of Bacterial Infection and Enhanced Osteoinductivity of a Hybrid Coating with Selective Silver Toxicity.
Xie Kai,Zhou Ziao,Guo Yu,Wang Lei,Li Guoyuan,Zhao Shuang,Liu Xiangmei,Li Jun,Jiang Wenbo,Wu Shuilin,Hao Yongqiang
Advanced healthcare materials
Antibacterial and osteogenic design is required for ideal orthopedic implants. The excellent antimicrobial performance of silver nanoparticles (AgNPs) has attracted interest for the treatment of implant-related infections. However, the dose-dependent cytotoxicity of silver and its negative impact on bone implants restrict the further use of AgNPs coatings. Therefore, a hybrid coating containing polydopamine (PDA), hydroxyapatite (HA), AgNPs, and chitosan (CS) is prepared. Organic chelators CS and PDA that have promising biocompatibility are used to prevent the rapid release of silver ions from the AgNPs coating. The double chelating effect of PDA and CS significantly reduces silver ion release from the hybrid coating. The coating exhibits excellent anti-biofilm efficiency of 91.7%, 89.5%, and 92.0% for Staphylococcus aureus, Staphylococcus epidermidis, and Escherichia coli, respectively. In addition, the coating can significantly stimulate osteogenic differentiation of MC3T3-E1 cells and promote bone-implant osseointegration in vivo as compared to that in the control group. The longitudinal biosafety of the coating is confirmed in vivo by histological evaluation and blood tests. The results of this study indicate that the hybrid coating exhibits antibacterial properties as well as allow bone-implant osseointegration, thereby providing insight into the design of multifunctional implants for long-term orthopedic applications.
Mussel-inspired hybrid coating functionalized porous hydroxyapatite scaffolds for bone tissue regeneration.
Han Lu,Jiang Yanan,Lv Chen,Gan Donglin,Wang Kefeng,Ge Xiang,Lu Xiong
Colloids and surfaces. B, Biointerfaces
The scaffold for bone tissue engineering should possess proper porosity, adequate mechanical properties, cell affinity for cell attachment, and the capability to bind bioactive agents to induce cell differentiation. In this study, we successfully prepared a porous hydroxyapatite (HA) scaffold that is functionalized by poly(L-lysine)/polydopamine (PLL/PDA) hybrid coating. The PLL/PDA coating takes advantages of the high protein and cell affinity of PDA, as well as the biodegradability of PLL. Therefore, the coating can anchor bone morphogenic protein-2 (BMP2) to the HA scaffold via catechol chemistry under a mild condition so as to protect the bioactivity of BMP2. Meanwhile, the coating can also release BMP2 in a tunable and sustainable manner as the PLL degrades in the physiological environment. The BMP2-entrapped PLL/PDA coating on the HA scaffold can more efﬁciently promote osteogenic differentiation of bone marrow stromal cells (BMSCs) in vitro and induce ectopic bone formation to a much greater level in vivo compared with a bare HA scaffold that delivers BMP2 in a burst manner. All of these results suggest that the PDA-mediated catechol modification of the HA scaffold can be an effective strategy to develop sustainable protein delivery system, and that the PLL/PDA-coated HA scaffold could be a promising candidate for bone tissue engineering applications.
Antibacterial Properties of Mussel-Inspired Polydopamine Coatings Prepared by a Simple Two-Step Shaking-Assisted Method.
Kord Forooshani Pegah,Polega Elizabeth,Thomson Kevin,Bhuiyan Md Saleh Akram,Pinnaratip Rattapol,Trought Mikhail,Kendrick Chito,Gao Yuesheng,Perrine Kathryn A,Pan Lei,Lee Bruce P
Frontiers in chemistry
A simple two-step, shaking-assisted polydopamine (PDA) coating technique was used to impart polypropylene (PP) mesh with antimicrobial properties. In this modified method, a relatively large concentration of dopamine (20 mg ml) was first used to create a stable PDA primer layer, while the second step utilized a significantly lower concentration of dopamine (2 mg ml) to promote the formation and deposition of large aggregates of PDA nanoparticles. Gentle shaking (70 rpm) was employed to increase the deposition of PDA nanoparticle aggregates and the formation of a thicker PDA coating with nano-scaled surface roughness (RMS = 110 nm and Ra = 82 nm). Cyclic voltammetry experiment confirmed that the PDA coating remained redox active, despite extensive oxidative cross-linking. When the PDA-coated mesh was hydrated in phosphate saline buffer (pH 7.4), it was activated to generate 200 μM hydrogen peroxide (HO) for over 48 h. The sustained release of low doses of HO was antibacterial against both gram-positive () and gram-negative () bacteria. PDA coating achieved 100% reduction (LRV ~3.15) when incubated against and 98.9% reduction (LRV ~1.97) against in 24 h.
Mechanical Enhancement of Bioinspired Polydopamine Nanocoatings.
Malollari Katerina G,Delparastan Peyman,Sobek Caroline,Vachhani Shraddha J,Fink Tanner D,Zha R Helen,Messersmith Phillip B
ACS applied materials & interfaces
Inspired by the catechol and amine-rich adhesive proteins of mussels, polydopamine (pDA) has become one of the most widely employed methods for functionalizing material surfaces, powered in part by the versatility and simplicity of pDA film deposition that takes place spontaneously on objects immersed in an alkaline aqueous solution of dopamine monomer. Despite the widespread adoption of pDA as a multifunctional coating for surface modification, it exhibits poor mechanical performance. Attempts to modify the physical properties of pDA by incorporation of oxidizing agents, cross-linkers, or carbonization of the films at ultrahigh temperatures have been reported; however, improving mechanical properties with mild post-treatments without sacrificing the functionality and versatility of pDA remains a challenge. Here, we demonstrate thermal annealing at a moderate temperature (130 °C) as a facile route to enhance mechanical robustness of pDA coatings. Chemical spectroscopy, X-ray scattering, molecular force spectroscopy, and bulk mechanical analyses indicate that monomeric and oligomeric species undergo further polymerization during thermal annealing, leading to fundamental changes in molecular and bulk mechanical behavior of pDA. Considerable improvements in scratch resistance were noted in terms of both penetration depth (32% decrease) and residual depth (74% decrease) for the annealed pDA coating, indicating the enhanced ability of the annealed coating to resist mechanical deformations. Thermal annealing resulted in significant enhancement in the intermolecular and cohesive interactions between the chains in the pDA structure, attributed to cross-linking and increased entanglements, preventing desorption and detachment of the chains from the coating. Importantly, improvements in pDA mechanical performance through thermal annealing did not compromise the ability of pDA to support secondary coating reactions as evidenced by electroless deposition of a metal film adlayer on annealed pDA.