ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Lan Tang,Sining Zhou,Fan Li,Lianpeng Sun,Hui Lu
The efficient and selective removal of refractory antibiotics from high-strength antibiotic production wastewater is crucial but remains a substantial challenge. In this study, a novel ozone micronano-bubble (MNB)-enhanced treatment system was constructed for antibiotic production wastewater treatment. Compared with conventional ozone, ozone MNBs exhibit excellent treatment efficiency for oxytetracycline (OTC) degradation and toxicity decrease. Notably, this study identifies the overlooked singlet oxygen (1O2) for the first time as a crucial active species in the ozone MNB system through probe and electron paramagnetic resonance methods. Subsequently, the oxidation mechanisms of OTC by ozone MNBs are systematically investigated. Owing to the high reactivity of OTC toward 1O2, ozone MNBs enhance the selective and anti-interference performance of OTC degradation in raw OTC production wastewater with complex matrixes. This study provides insights into the mechanism of ozone MNB-enhanced pollutant degradation and a new perspective for the efficient treatment of high-concentration industrial wastewater using ozone MNBs. In addition, this study presents a promising technology with scientific guidance for the treatment of antibiotic production wastewater.
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 35
·6777-6783
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IF 7.571
Jixiang Wang,Xiaolei Li,Rong Zhang,Bingjie Fu,Mingcan Chen,Mengxue Ye,Wanyu Liu,Jingjing Xu,Guoqing Pan,Hongbo Zhang
The detection and elimination of antibiotic contaminants, such as oxytetracycline (OTC), a broad-spectrum tetracycline antibiotic, would be of help in efficient environmental monitoring, agriculture and food safety tests. Nevertheless, currently available methodologies, which mostly rely on the chromatographic separation of OTC, suffer from low sensitivity and complicated processes. Thus, we report here on the design and synthesis of a fluorescent sensor based on molecularly imprinted magnetic halloysite nanotubes (referred to as MHNTs@FMIPs) for the effective detection and purification of OTC in actual environmental samples. The fluorescence of the MHNTs@FMIPs was quenched obviously upon loading with OTC, covering a linear concentration range of 10–300 nM with a limit of detection (LOD) as low as 8.1 nM. The imprinting factor is 4.47, indicating an excellent specificity. Furthermore, the MHNTs@FMIPs can be applied to the quantitative detection of OTC (5 cycles of 300 nM) in aquaculture wastewater and Yangtze River water, demonstrating their immense application potential.
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CHEMOSPHERE
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2022
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IF 8.943
Yu Wang,Xinye Gong,Deying Huang,Shuwen Yan,Jibiao Zhang
Surface water contains a large amount of dissolved organic matter (DOM). Interactions between DOM and micropollutants have a significant impact on micropollutant degradation. In this study, algal extracellular polymeric substances (EPS) and natural organic matter (NOM) were selected as two DOM sources and oxytetracycline (OTC) as a representative micropollutant. EPS was mainly composed of tryptophan and protein-like organics, while NOM was mainly composed of fulvic acid-like, humic acid-like, and hydrophobic acid components. In addition, OTC degradation significantly decreased when bound with EPS and the C=O and C–H bonds of CH 2 or CH 3 groups may be involved in binding EPS and OTC, respectively, while –COOH may be involved in the binding of NOM and OTC. Furthermore, triplet intermediates were found to play a major role in OTC photodegradation in both EPS and NOM, with the contribution calculated as 49.96% and 44.61%, respectively. Steady-state concentrations of 3 EPS* in EPS and 3 NOM* in NOM were 3.59 × 10 −14 mol L −1 and 5.54 × 10 −15 mol L −1 , respectively. These results provide new insights into the degradation of antibiotic-containing wastewater in the natural environment or engineering applications.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
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IF 8.91
Xiaoying Jin,Heng Li,Xiuduan Zhu,Na Li,Gary Owens,Zuliang Chen
The integration of metal–organic frameworks with other functional materials has recently emerged as a promising approach for creating innovative materials for environmental remediation. Here, a nano-sized iron/nickel (Fe/Ni) functionalized zeolitic imidazolate framework-8 (ZIF-8-Fe/Ni) was fabricated for oxytetracycline (OTC) removal from wastewater. Cyclic voltammetry and amperometric I-t measurements indicated that OTC was degraded by ZIF-8-Fe/Ni. X-ray diffraction spectroscopy (XRD), transmission electron microscopy mapping (TEM-mapping) and X-ray photoelectron spectroscopy (XPS) indicated that Fe/Ni was evenly dispersed throughout ZIF-8 and partially oxidized after reaction with OTC. OTC adsorption isotherms and kinetics best fitted the Langmuir isotherm ( R 2 > 0.982) and pseudo-second-order model ( R 2 > 0.997), respectively. Reduction kinetics data followed the pseudo-first-order model ( R 2 > 0.905), where the apparent activation energy ( E a) was 22.9 kJ mol −1 , demonstrating that OTC degradation was mainly via a chemical process. The practical removal efficiency of OTC from real wastewater by ZIF-8-Fe/Ni was 92.6%, where even after application of ZIF-8-Fe/Ni for 5 consecutive removal cycles, a high OTC removal of 74.9% was maintained. Thus ZIF-8-Fe/Ni exhibited both high removal efficiency and good recyclability .
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Journal of Environmental Chemical Engineering
·
2022
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IF 7.968
Jingzhen Wang,Linlin Zang,Libin Wang,Yutong Tian,Zhiyu Yang,Yumei Yue,Liguo Sun
Photocatalytic degradation is an effective technique for removing antibiotics from contaminated water . The kernel of photocatalytic degradation lies in the design and preparation of high-performance and recyclable catalysts. Herein, magnetic porous cobalt ferrite/reduced graphene oxide (CF/rGO) balls were prepared by calcination of spherical composites obtained via modified microfluidic method for effective photocatalytic degradation of oxytetracycline (OTC). The strong interfacial interaction between rGO and cobalt ferrite nanoparticles in porous balls enhanced electron transfer , charge separation and light absorption . Porous spherical structure was favorable for light harvesting. The catalyst could rapidly and efficiently absorb OTC. These characteristics were beneficial to the enhancement of photocatalytic efficiency. The optimized sample (CF/rGO-0.2) exhibited an excellent apparent rate constant (0.0410 min −1 ) for OTC degradation under visible light irradiation, which was 3.73 times that of CF/rGO-0 (0.0110 min −1 ). CF/rGO-0.2 had excellent stability in cycle experiments and could be quickly recovered by magnets. The trapping experiments showed that hole (h + ) and superoxide radicals (·O 2 - ) acted an extremely important role in degradation of OTC, thus suggesting a possible photocatalytic reaction mechanism. This work provides a potential photocatalyst for antibiotic removal from water.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Chengdong Shi,Shuyan Yu,Le Wang,Xiuling Zhang,Xiaoqiu Lin,Congju Li
The treatment of antibiotic wastewater is a hot research topic now. To achieve a fast and efficient degradation effect, aligned polyacrylonitrile-based carbon nanofibrous (ACFs) membrane as anodic electrocatalysis microfiltration membrane was fabricated by high-speed electrospinning technology in this work. The morphology, structure, electrochemical performance and mechanical properties of ACFs membrane as anode filter were characterized. The high degrees of nanofiber alignment and carbonization are obtained at the rotating speed of 1500 r/min and the temperature of 900 ℃, respectively, which provides the ACFs membrane with good electrical conductivity and mechanical properties. The highest removal rate (nearly 80%) of tetracycline/oxytetracycline (TC/OTC) in mixture solution was obtained with 4 layers of ACFs membranes under the potential of 2.5 V at the initial concentration of 40 mg/L within the reaction time of 120 min. A decrease of removal rate by only 5% after 5 cycles of repeated experiments indicated good electrocatalytic activity and cycling stability of ACFs membrane. These results indicated that more than one antibiotic could be treated rapidly by ACFs membranes with a high removal rate in a short reaction time, and has great application prospects in the treatment of refractory antibiotic wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Ning An,Min Zhao,Xiangyong Zheng,Qi Wang,Xianfeng Huang,Bo Sun,Yi Shen,Jun Wang,Baoliang Chen,Renlan Liu
Metal-free carbonaceous catalysts are receiving increasing attention in wastewater treatment . Here, nitrogen and sulfur co-doped carbon sphere catalysts (N,S-CSs 900 -OH) were synthesized using glucose and L -cysteine via a hydrothermal method and high temperature alkali activation. The N,S-CSs 900 -10%-OH exhibited excellent catalytic performance for the degradation of oxytetracycline (OTC). The degradation rate was 95.9% in 60 min, and the reaction equilibrium rate constant was 0.0735 min −1 ( k 0–15 min ). The synergistic effect of adsorption-promoting degradation was demonstrated in the removal process of OTC. The excellent adsorption capacity of N,S-CSs 900 -10%-OH ensured the efficient oxidation of OTC. N,S-CSs 900 -10%-OH reduced the activation energy of the OTC degradation reaction ( E a=18.23 kJ/mol). Moreover, the pyrrolic N, thiophene S and carbon skeleton played an important role in the degradation of OTC based on density function theory, and the catalytic mechanism was expounded through radical and nonradical pathways. The active species involved in the reaction were O 2 •− , 1 O 2 , SO 4 •− and •OH, of which O 2 •− was the primary reactive species. This study provides a new insight into the reaction mechanism for efficient treatment of organic pollutants using metal-free doped porous carbon materials.
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ANALYTICA CHIMICA ACTA
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2021
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IF 6.558
Weihang Wang,Chi Zhang,Jiaxin Guo,Gaiping Li,Baoxian Ye,Lina Zou
Here, we developed a homogeneous electrochemical biosensor for the sensitive determination of antibiotic by the CHA reaction and the consecutive adenine mediated probe fixation. The binding of target to the target recognition sequences in the triple-helix DNA can release the trigger. It can initiate the catalytic hairpin assembly (CHA) to generate lots of mimic targets, which were labeled with electroactive substance ferrocene (Fc). Because the generated mimic target has consecutive sequence of adenines (PolyA), they can be self-assembled on the AuNPs modified electrode and finally realize electrochemical detection . Under optimal conditions, this developed biosensor achieved a satisfactory limit of detection of 0.089 nM (S/N = 3) and a linear range from 0.1 nM to 100 nM for sensitive detection of oxytetracycline with good specificity. The whole process is carried out in homogeneous solution, not only realizes signal amplification, but also avoids the complex modification process of electrode surface. Compared with some reported electrochemical sensors , the method is easier to operate and has good precision.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Ying Sun,Xuejiang Wang,Siqing Xia,Jianfu Zhao
Biodegradable plastics have been evaluated as promising alternatives for conventional polymers in various fields. Although microplastics (MPs) have been reported as vectors for pollutants in the environment ( e.g. antibiotics), knowledge about the chemicals carrying mechanisms of degradable MPs during the biodegradation process is limited. In this study, we investigated the adsorption behavior of oxytetracycline (OTC) on polylactic acid (PLA) MPs during its biodegradation process. Scanning electron microscopy (SEM) discovered the growth of scattered rod-shaped bacteria on the surface of PLA MPs. Two-dimensional correlation spectroscopy (2D-COS) combined with Fourier transform infrared spectroscopy (FTIR) identified the breakage of ester linkages and the generation of more oxygen-containing functional groups, indicating PLA biodegradation occurred. The presence of a biofilm coating increased the OTC adsorption capacity on MPs by 20.15%, mainly due to OTC complexing with chemical functional groups existing in biofilms ( e.g. N–H functional group). More oxygen-containing functional groups were exposed on the surface of PLA MPs after removing biofilms, which further increased the adsorption quantity of OTC by 39.01% through enhanced hydrogen bonding compared with biofilm coating MPs. The adsorption quantity of OTC adsorbed onto MPs first increased and then decreased with the pH ranging from 3.0 to 9.0, which was dominated by electrostatic interaction and hydrophobic interaction. In addition, the adsorption capacity of MPs was suppressed by the presence of fulvic acid (FA) due to that the adsorbed FA blocked further OTC adsorption and OTC showed higher affinity to free FA compared with MPs. These results unravel the OTC adsorption behavior of PLA MPs undergoing microbial adhesion and degradation, which could be useful for understanding the environmental sorption behavior of degradable MPs.
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Nanomaterials
·
2023
·Vol. 13
·期 20
·2764
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IF 5.3
Muneerah Alomar,Naila Arshad,Muhammad Sultan Irshad,Shaimaa A. M. Abdelmohsen,Iftikhar Ahmed,Nawal Alhoshani,Areej S. Alqarni
Developing a sustainable environment requires addressing primitive water scarcity and water contamination. Antibiotics such as oxytetracycline (OTC) may accumulate in the environment and in the human body, increasing the risks to the ecosystem. The treatment of polluted water and the production of potable water can be achieved in a variety of ways, including photodegradation, solar distillation, and filtration. Freshwater supplies can be increased by implementing energy-efficient technologies for the production of clean water. Solar water evaporation combined with photocatalytic degradation and sterilization offers a promising avenue for integration into the clean water and energy production fields. The present study reports the synthesis of a 3D solar steam generator comprised of BiVO4and carbon nanotubes (CNT) nanocomposite decorated over a cigarette filter as the light-to-heat conversion layer for solar steam generation. The BiVO4@CNT-based 3D solar evaporator over the hydrophilic cellulosic fibers of the cigarette filter endowed excellent evaporation rates (2.36 kg m−2h−1) under 1 kW m−2solar irradiation, owing to its superior hydrophilicity and broadband solar absorption (96%) equipped with localized heating at microscale thermal confinement optimized by the minimum thermal conductivity of the overall system. Furthermore, the BiVO4@CNT composite exhibited a heightened photo activity up to 83% of the photodegradation of oxytetracycline (OTC) antibiotic due to the inhibition of charge recombination from the industrial effluents. This approach transforms the water-energy nexus into a synergistic bond that offers opportunities to meet expected demand, rather than being competitive.Keywords:solar evaporation;BiVO4;MWCNTs;photocatalytic;freshwater;oxytetracycline
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WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 10
·1-14
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IF 2.9
Jia Wenqiang,Pan Xiangrui,Song Jiaying,Wang Jian,Sun Weikai,Xin Yanjun,Yan Qinghua,Zhou Chengzhi,Zheng Hao,Liu Guocheng
Physical disintegration of macro biochars in natural environments produces nano biochars, thus affecting environmental processes (e.g., adsorption, migration) of antibiotic contaminants. However, knowledge about the relationships between adsorption behaviors of antibiotics and unique physicochemical colloidal properties of nano biochar are relatively limited. In this study, a nano biochar (NSD700) was prepared from sawdust-derived biochar (SD700) by a combination method of ball milling, sonication, and centrifugation to contrastively investigate their adsorption for oxytetracycline (OTC). NSD700 had similar chemical structure properties of carbon fraction with SD700, whereas NSD700 possessed greater surface area and porosity. The maximal sorption capacity of OTC on NSD700 was 30.7 mg/g, ~3 times greater than that of SD700 (10.4 mg/g), primarily benefiting from more exposed surfaces and pores. OTC adsorption on NSD700 was inhibited under acidic and alkaline condition, and the inhibiting effect was more significant in comparison with that on SD700. OTC sorption onto NSD700 gradually decreased with increasing concentration of Na + , but was not observed for SD700. Aggregation kinetic of NSD700 varying with Na + concentration demonstrated that the inhibiting effect might be affiliated with the destabilization and aggregation of NSD700, which could obstruct adsorption sites. This study provided insights for antibiotic adsorption characteristics on nano biochar and will help understanding the process and fate of antibiotics in the biochar-remediated environment. Graphical Abstract
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WATER RESEARCH
·
2023
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IF 12.8
Yinhan Jin,Jiuyan Chen,Qiang Zhang,Usman Farooq,Taotao Lu,Bin Wang,Zhichong Qi,Weifeng Chen
Herein, the influences of rhamnolipid (a typical biosurfactant) on oxytetracycline (OTC) transport in the porous media and their variations with the surface heterogeneities of the media (uncoated sand, goethite (Goe)-, and humic acid (HA)-coated sands) were explored. Compared to uncoated sand, goethite and HA coatings suppressed OTC mobility by increasing deposition sites. Interestingly, rhamnolipid-affected OTC transport strongly depended on the chemical heterogeneities of aquifers and biosurfactant concentrations. Concretely, adding rhamnolipid (1–3 mg/L) inhibited OTC mobility through sand columns because of the bridging effect of biosurfactant between sand and OTC. Unexpectedly, rhamnolipid of 10 mg/L did not further improve the inhibition of OTC transport owing to the fact that the deposition capacity of rhamnolipid reached its maximum. OTC mobility in Goe-coated sand columns was inhibited by 1 mg/L rhamnolipid. However, the inhibitory effect decreased with the increasing rhamnolipid concentration (3 mg/L) and exhibited a promoted effect at 10 mg/L rhamnolipid. This surprising observation was that the increased rhamnolipid molecules gradually occupied the favorable deposition sites (i.e., the positively charged sites). In comparison, rhamnolipid facilitated OTC transport in the HA-coated sand column. The promotion effects positively correlated with rhamnolipid concentrations because of the high electrostatic repulsion and deposition site competition induced by the deposited rhamnolipid. Another interesting phenomenon was that rhamnolipid's enhanced or inhibitory effects on OTC transport declined with the increasing solution pH because of the decreased rhamnolipid deposition on porous media surfaces. These findings benefit our understanding of the environmental behaviors of antibiotics in complex soil-water systems containing biosurfactants.
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