Role of moderately hydrophobic chitosan flocculants in the removal of trace antibiotics from water and membrane fouling control.
Yang Zhen,Hou Tianyang,Ma Jiangya,Yuan Bo,Tian Ziqi,Yang Weiben,Graham Nigel J D
Water research
In this paper we describe the preparation and testing of a new class of chitosan-based flocculants for the treatment of surface waters containing antibiotic compounds. Three forms of moderately hydrophobic chitosan flocculants (MHCs) were prepared by chemically grafting hydrophobic branches with different lengths onto hydrophilic chitosan and these were evaluated by jar tests and a bench-scale continuous flow ultrafiltration (UF) membrane process with coagulation/sedimentation pre-treatment. Tests were conducted using both synthetic and real surface water in which norfloxacin and tylosin were added as representative antibiotics at an initial concentration of 0.1 μg/L. In jar tests, the MHCs achieved similar high removal efficiencies (REs) of turbidity and UV absorbance, but much higher REs of the two antibiotics (71.7-84.7% and 68.7-76.6% for synthetic and river waters, respectively), compared to several commercial flocculants; the superior performance was attributed to an enhanced hydrophobic interaction and H-bonding between the flocculants and antibiotics. The presence of suspended kaolin particles and humic acid enhanced the antibiotic removal, speculated to be through MHC bridging of the kaolin/humic acid and antibiotic molecules. In the continuous flow tests involving flocculation/sedimentation-UF for 40 days, an optimal MHC achieved a much greater performance than polyaluminium chloride in terms of the overall removal of antibiotics (RE (norfloxacin) of ∼90% and RE (tylosin) of ∼80%) and a greatly reduced rate of membrane fouling; the latter resulting from a more porous and looser structure of cake layer, caused by a surface-modification-like effect of residual MHC on the hydrophobic PVDF membrane. The results of this study have shown that MHCs offer a significant advance over the use of existing flocculants for the treatment of surface water.
10.1016/j.watres.2020.115775
Adsorption of tetracycline in aqueous solution by biochar derived from waste Auricularia auricula dregs.
Dai Yingjie,Li Jingjing,Shan Dexin
Chemosphere
This study investigated the adsorption of tetracycline (TC) on biochar (BC) derived from waste Auricularia auricula dregs obtained at different pyrolysis temperatures. The characterization of BC and batch experiment results showed that BC prepared at a higher temperature was more suitable for removing TC, where the maximum adsorption capacities of BC samples prepared at 300 °C, 500 °C, and 700 °C were 7.22 mg/g, 9.90 mg/g, and 11.90 mg/g, respectively. A pseudo-first order kinetics model and Freundlich, Temkin, and Dubinin-Radushkevich isotherm models fitted well to the adsorption data. Liquid film diffusion was the rate-controlling step. In addition, π-π electron donor-acceptor interactions may have played a dominant role in the adsorption mechanism between the enone structure of TC and aromatic C of BC. These results may facilitate further investigations of the adsorption mechanism and optimization of the process.
10.1016/j.chemosphere.2019.124432
Chitosan modified N, S-doped TiO and N, S-doped ZnO for visible light photocatalytic degradation of tetracycline.
Farhadian Negin,Akbarzadeh Rokhsareh,Pirsaheb Meghdad,Jen Tien-Chien,Fakhri Yadolah,Asadi Anvar
International journal of biological macromolecules
N, S-doped TiO (NST), N, S-doped ZnO (NSZ) and their composite with chitosan (NST/CS, NSZ/CS) were synthesized by sol gel-hydrothermal method. The prepared samples were characterized using XRD, FTIR, TEM and BET techniques. These photocatalysts were used for the photocatalytic degradation of tetracycline under visible light irradiation. At screening test, NST/CS had the highest tetracycline degradation efficiency of 91% for duration of 20 min under visible light. The blending of chitosan with NST increases the rate of photocatalytic degradation of tetracycline about 2 times. A detail characterization including HRTEM, SEM, EDS and DRS were conducted for NST/CS, the most active photocatalyst in this study. Photocatalytic activity test was conducted by varying tetracycline concentration, irradiation time, catalyst's concentration and pH using response surface methodology to find out the optimum condition for photocatalytic activity. The reusability of as-synthesized NST/CS was assessed which due to its high recoverability can be applied as an effective catalyst for degradation of organic substances in water and wastewater especially for degradation of emerging pollutants such pharmaceutical pollutants. The results from this work show a promising material for local authorities and pharmaceutical facilities to use for the treatment of pharmaceutical pollutants and tetracycline removal in water resource.
10.1016/j.ijbiomac.2019.03.217
Visible-light-driven removal of tetracycline antibiotics and reclamation of hydrogen energy from natural water matrices and wastewater by polymeric carbon nitride foam.
Wang Hou,Wu Yan,Feng Mingbao,Tu Wenguang,Xiao Tong,Xiong Ting,Ang Huixiang,Yuan Xingzhong,Chew Jia Wei
Water research
Water and energy are key sustainability issues that need to be addressed. Photocatalysis represents an attractive means to not only remediate polluted waters, but also harness solar energy. Unfortunately, the employment of photocatalysts remains a practical challenge in terms of high cost, low efficiency, secondary pollution and unexploited water matrices influence. This study investigated the feasibility of photocatalysis to both treat water and produce hydrogen with practical water systems. Polymeric carbon nitride foam (CNF) with large surface area and mesoporous structure was successfully prepared via the bubble-template effect of ammonium chloride decomposition during thermal condensation. The reaction kinetics, mechanisms, and effect of natural water matrices and wastewater on CNF-based photocatalytic removal of tetracycline hydrochloride (TC-HCl) were systematically investigated. Furthermore, the efficiency of clean hydrogen energy from natural water matrices and wastewater was also evaluated. It was found that the photocatalytic performance of CNF for TC-HCl removal was principally affected by calcination temperature in the presence of NHCl. The degradation rates of CNF-4 (calcined at 550 °C) were approximately 1.84, 2.49 and 7.47 times than that of the CNF-2 (calcined at 600 °C), CNF-1 (calcined at 500 °C) and GCN (without NHCl), respectively. Results indicate that the improved photocatalytic performance was predominantly ascribed to the large specific surface area, increased availability of exposed active sites, and enhanced transport and separation efficiency of the photogenerated carrier. Based on electron spin resonance, chemical trapping experiment and density functional theory calculation, photoinduced oxidizing species (·O and holes) initially attacked the C-N-C fragment of TC molecules, which were finally mineralized to CO, water and inorganic matters. Under the synergistic influence of water constituents (including acidity and alkalinity, ion species and dissolved organic substances), various water matrices greatly affected the degradation rate of TC-HCl, with the highest removal efficiency of 78.9% in natural seawater, followed by reservoir water (75.0%), tap water (62.3%), deionized water (49.8%), reverse osmosis concentrate (32.7%) and pharmaceutical wastewater (18.9%). Interestingly, low amounts of the emerging microplastics slightly improved TC-HCl removal, whereas high amounts (1.428 × 10 P/cm) restricted removal due to light absorption and the intrinsic adsorption interaction. Moreover, the photocatalysts were able over repeated usage. Notably, the hydrogen yields rates of polymeric carbon nitride foam were 352.2, 299.8, 184.9 and 94.3 μmol/g/h in natural seawater, pharmaceutical wastewater, water from reservoir and tap water, respectively. This study proves the potential of novel nonmetal porous photocatalyst to simultaneously treat wastewater while converting solar energy into clean hydrogen energy.
10.1016/j.watres.2018.07.025
Simultaneous removal of antibiotics and antibiotic resistance genes from pharmaceutical wastewater using the combinations of up-flow anaerobic sludge bed, anoxic-oxic tank, and advanced oxidation technologies.
Hou Jie,Chen Zeyou,Gao Ju,Xie Yonglei,Li Linyun,Qin Songyan,Wang Qing,Mao Daqing,Luo Yi
Water research
Pharmaceutical wastewater often contains high levels of antibiotic residues and serves as an important reservoir for antibiotic resistance genes (ARGs). However, the current pharmaceutical wastewater treatment plants (PWWTPs) were not sufficiently effective in removing antibiotics and ARGs. Here, we designed a lab-scale simulation reactor, including up-flow anaerobic sludge bed (UASB), anoxic-oxic tank (A/O), and four separate advanced oxidation processes (AOPs) i.e., UV, Ozonation, Fenton, and Fenton/UV, to simultaneously remove 18 antibiotics and 10 ARGs from a real pharmaceutical wastewater. The results showed that all antibiotics were fully eliminated through the reactor during 180 d-operation. Among all treatment units, UASB provided the greatest contribution (85.8 ± 16.1%) for the removal of 18 antibiotics. The mass balance results manifested that degradation was a predominant mechanism for the removal of tetracyclines, sulfamethoxazole, and ampicillin (62.5-80.9%), while sorption to sludge (73.9%) was predominant for enrofloxacin removal in UASB. Meanwhile, the substantial decrease of ARG absolute abundance (log reduction by 0.1-3.1 fold) through the whole reactor was observed although the existence of the partial enrichment (1.2-3.8 log units) from the influent to the A/O unit. Fenton/UV combination was the most effective AOP for the removal of ARGs. Finally, the optimum operating conditions for the removal of ARGs using Fenton was also proposed considering the relatively lower cost and high ARG elimination. Overall, this study provides feasible suggestions for the design of real PWWTPs for simultaneous removal of antibiotics and ARGs.
10.1016/j.watres.2019.05.034
FeO accelerates tetracycline degradation during anaerobic digestion: Synergistic role of adsorption and microbial metabolism.
Zhao Zisheng,Zhang Guangyi,Zhang Yaobin,Dou Ming,Li Yang
Water research
Antibiotics contaminants, for example, tetracycline (TC) in the environment have attracted extensive attention around the world, and appropriate treatments for such contaminants are urgently required. In this study, five groups of anaerobic reactors supplemented with different amounts of FeO were operated periodically to investigate their performance on TC removal. The results showed that FeO effectively promoted TC removal. Compared with the control reactor, the TC removal efficiency was increased by 7.3% when co-digested with glucose, and increased by 40.4% when mono TC was digested in reactors with 5.0 g/L FeO. Further analysis indicated that the probable mechanism of FeO promoting TC removal was through TC being adsorbed from the liquid onto FeO, making TC more available for microbes to be biodegraded. Microbial community analysis indicated that the bacteria (Klebsiella, Pseudomonas, and Escherichia) related to TC removal were enriched, which meant more pathways for TC removal were available following the addition of FeO. In addition, in the FeO-supplemented reactors, syntrophic metabolism (between Desulfovibrio and Methanobacterium, Azonexus and Methanobacterium) were possibly established, which played an important role in improving TC removal and CH production. The electron transport system data further confirmed these results. The functional gene classification for Kyoto Encyclopedia of Genes and Genomes (KEGG) analysis demonstrated that the dominant functions enhanced by FeO supplementation was microbial metabolic activities.
10.1016/j.watres.2020.116225
Mitigating antibiotic pollution using cyanobacteria: Removal efficiency, pathways and metabolism.
Pan Minmin,Lyu Tao,Zhan Lumeng,Matamoros Victor,Angelidaki Irini,Cooper Mick,Pan Gang
Water research
The occurrence of pharmaceuticals and personal care products (PPCPs) in wastewater poses huge environmental threats, even at trace concentrations, and novel approaches are urged due to the inefficiencies of conventional wastewater treatment plants, especially when processing contaminants at high concentrations. Meanwhile, another widespread problem in the aquatic domain is the occurrence of harmful algal blooms (HABs) which cause serious damage to the ecosystem, but have rarely been investigated for possible valorization. This study investigated the possibilities, mechanisms, and effects of toxin release of using a harmful cyanobacterial species, Microcystis aeruginosa (M. aeruginosa), in order to remove the widely used drug, tetracycline, at high concentration. The results were compared with the performance obtained by the use of the hitherto generally-selected chlorophyte alga Chlorella pyrenoidosa (C. pyrenoidosa) for tetracycline concentrations of 10-100 mg L. M. aeruginosa exhibited a much more effective and rapid tetracycline removal (over 98.0% removal in 2 days) than did C. pyrenoidosa (36.7%-93.9% in 2 days). A comprehensive kinetic investigation into probable removal pathways indicated that, theoretically, bio-remediation dominated the process by M. aeruginosa (71.6%), while only accounting for 20.5% by C. pyrenoidosa. Both microalgae promoted the hydrolysis of tetracycline under conditions of increased pH and inhibited abiotic photolytic reactions by the shading effect to the water column, when compared with control experiments. Although identical degradation by-products were identified from treatments by both microalgal species, distinct by-products were also confirmed, unique to each treatment. Moreover, the growth of M. aeruginosa biomass exhibited strong tolerance to tetracycline exposure and released significantly lower levels of microcystin-LR, compared with the control systems. This study supports the possibility of reusing HABs species for the effective remediation of antibiotics at high concentrations. We have further suggested possible mechanisms for remediation and demonstrated control of toxin release.
10.1016/j.watres.2020.116735