ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 21
·60704-60716
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IF 5.8
Zhang Nizi,Tang Chenliu,Bi Weixia,Sun Zhirong,Hu Xiang
Efficient removal of antibiotics from the aquatic environment is urgently needed due to their obstinate accumulation and non-biodegradability. In this study, a mesoporous carbon material (ZC-0.5) was successfully synthesized for the adsorption of sulfamethoxazole (SMX), one of the major antibiotics for the treatment of human and animal infections. ZIF-8 as the precursor of ZC-0.5, specifically, using cetyl trimethyl ammonium bromide (CTAB) and sodium laurate (SL) as dual templates and carbonizing at 800 ℃. This novel adsorbent exhibited a high proportion of mesopore (75.64%) and a large specific surface area (1459.73 m 2 ·g −1 ). The adsorption experiment examined the reusability of ZC-0.5 and that it could retain superior maximum adsorption capacities (167.45 mg∙L −1 ) after five cycles of adsorption and desorption. The adsorption process satisfied the pseudo-second-order kinetic (PSO) and mixed first- and second-order kinetic (MOE). It also satisfied the Freundlich and Sips isotherm models. Moreover, thermodynamic calculation indicated the adsorption process was spontaneous, endothermal, and entropy-increasing. Furthermore, plausible adsorption mechanisms were explained through van der Waals force, electrostatic interaction, hydrophobic force, π-π interaction, and hydrogen bond. This work offers a new efficient adsorbent for antibiotic elimination.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Xiaoli Su,Feiyun Sun,Jianjun Zhang,Dingyu Xing,Xiaoying Li,Zi Song,Liang Feng,Zhichao Huang,Ang Li
This study investigated the interaction between function microbiota succession and three electron acceptors in anaerobic sulfamethoxazole (SMX) degradation. Over 20%–60% SMX was degraded biologically after antibiotics acclimation under co-electron acceptors. Under sulfate- and nitrate-reducing conditions, SMX removal followed a pseudo-zero-order kinetic model and related to the sludge adsorption site. Microbiological analyses showed syntrophic community, including autotrophic denitrifiyer, nitrate reducing-sulfate oxidizier, and heterotrophic denitrifier , were putative SMX reducers. As an electron acceptor, sulfate was more beneficial in degrading SMX and maintaining the system stability and the colony structure. However, autotrophic nitrate-reducing sulfate-oxidizing bacteria has a stronger substrate competition advantage than sulfate-reducing bacteria (SRB), resulting in invalid SMX degradation. Thus, for the system start-up, SRB and iron/sulfur-based denitrifier should be preferentially enriched with sulfate electron acceptors to assure the removals of antibiotics. These results uncovered crucial factors that may affect the fate of SMX and associated biochemicals in anaerobic degradation processes but were previously overlooked.
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Catalysts
·
2023
·Vol. 13
·期 1
·172
·
IF 3.9
Yandong Xu,Jianjun Liao,Linlin Zhang,Yakun Li,Chengjun Ge
Rational design of composite nanostructured photocatalytic systems with good sunlight absorption capacity and efficient charge separation and transfer ability is an urgent problem to be solved in photocatalysis research. Here, a ZnMn2O4decorated three-dimensional carbon nitride with O, C co-doping, and nitrogen defect composite photocatalytic system was prepared using a simple hydrothermal method and subsequent calcination method. For the photocatalytic reactions, the presence of heterostructures, C, O co-doping, and nitrogen defects greatly promotes the separation and transfer of charges at the semiconductor/semiconductor interface under the local electric field, thereby extending its service life. The photocatalytic degradation efficiency of sulfamethoxazole in water is as high as 94.3% under the synergistic effects, which is also suitable for the complex water environment. In addition, the synthesized photocatalyst has good chemical stability and recyclability. This study provides a new opportunity to solve the problem of environmental pollution.Keywords:multi-defective C3N4;ZnMn2O4;composite system;photocatalytic sulfamethoxazole degradation
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yueling Yu,Jia Yang,Baogang Zhao,Xinfei Fan,Yuanlu Xu,Yanming Liu
Nonradical-based peroxymonosulfate (PMS) activation has recently caught increasing attention due to its less susceptible to environmental interference in the complex water matrix, but the performance of activators still requires further development for efficient pollutants degradation in wastewater treatment . Herein, a novel Co-Ni bimetal oxide loaded biochar was fabricated to boost nonradical PMS activation for enhancing sulfamethoxazole (SMX) degradation. According to the results, the as-obtained catalyst exhibited excellent SMX degradation efficiency of 96.2% within 30 min through complete nonradical oxidation pathway (including both 1 O 2 and mediated electron transfer). Co was confirmed to be the active sites to generate 1 O 2 dominated nonradical pathway. The biochar acted as the porous material to achieve the electron transfer oxidation process, as well as Ni ensured sufficient electron transfer rate and bound Co active sites to prevent the leaching of metal ions . Meanwhile, the prepared Co-Ni bimetal oxide loaded biochar possessed a remarkable catalytic degradation durability in the complex water environment conditions and showed universality for various organic contaminants . This study offers a valuable clue on the rational design of novel catalyst to induce the nonradical pathway-based persulfate activation .
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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 107
·期 18
·5813-5827
·
IF 5
Wu Tong,Guo Sheng-Zhi,Zhu Hai-Zhen,Yan Lei,Liu Zhi-Pei,Li De-Feng,Jiang Cheng-Ying,Corvini Philippe François-Xavier,Shen Xi-Hui,Liu Shuang-Jiang
Abstract Sulfonamide antibiotics (SAs) are serious pollutants to ecosystems and environments. Previous studies showed that microbial degradation of SAs such as sulfamethoxazole (SMX) proceeds via a sad -encoded oxidative pathway, while the sulfonamide-resistant dihydropteroate synthase gene, sul , is responsible for SA resistance. However, the co-occurrence of sad and sul genes, as well as how the sul gene affects SMX degradation, was not explored. In this study, two SMX-degrading bacterial strains, SD-1 and SD-2, were cultivated from an SMX-degrading enrichment. Both strains were Paenarthrobacter species and were phylogenetically identical; however, they showed different SMX degradation activities. Specifically, strain SD-1 utilized SMX as the sole carbon and energy source for growth and was a highly efficient SMX degrader, while SD-2 did could not use SMX as a sole carbon or energy source and showed limited SMX degradation when an additional carbon source was supplied. Genome annotation, growth, enzymatic activity tests, and metabolite detection revealed that strains SD-1 and SD-2 shared a sad -encoded oxidative pathway for SMX degradation and a pathway of protocatechuate degradation. A new sulfonamide-resistant dihydropteroate synthase gene, sul918 , was identified in strain SD-1, but not in SD-2. Moreover, the lack of sul918 resulted in low SMX degradation activity in strain SD-2. Genome data mining revealed the co-occurrence of sad and sul genes in efficient SMX-degrading Paenarthrobacter strains. We propose that the co-occurrence of sulfonamide-resistant dihydropteroate synthase and sad genes is crucial for efficient SMX biodegradation. Key points
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Two sulfamethoxazole-degrading strains with distinct degrading activity, Paenarthrobacter sp. SD-1 and Paenarthrobacter sp. SD-2, were isolated and identified.
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Strains SD-1 and SD-2 shared a sad-encoded oxidative pathway for SMX degradation.
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A new plasmid-borne SMX resistance gene (sul918) of strain SD-1 plays a crucial role in SMX degradation efficiency.
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Environmental Science and Ecotechnology
·
2023
·
IF 12.6
Jing-Yan Zhang,Jie Ding,Lu-Ming Liu,Rui Wu,Lan Ding,Jun-Qiu Jiang,Ji-Wei Pang,Yan Li,Nan-Qi Ren,Shan-Shan Yang
Sulfamethoxazole (SMX) is a significant environmental concern due to its adverse effects and ecological risks. SMX elimination in aquatic environments via photocatalysis presents a viable solution, given its high oxidation potential. However, such a solution remains controversial, primarily due to a lack of selectivity. Here we introduce a molecularly imprinted TiO 2 @Fe 2 O 3 @g-C 3 N 4 (MFTC) photocatalyst designed for the selective degradation of SMX. To assess MFTC's selectivity, we applied it to degrade synthetic wastewater containing SMX alongside interfering species sulfadiazine (SDZ), ibuprofen (IBU), and bisphenol A (BPA). The results demonstrated a selective degradation efficiency rate of 96.8%, nearly twice that of competing pollutants. The molecularly imprinted sites within the catalyst played a crucial role by selectively capturing SMX and enhancing its adsorption, thereby improving catalytic efficiency. The degradation process involved •OH and •O 2 − free radicals, with a newly proposed double Z-scheme mechanism and potential pathway for SMX degradation by the MFTC photocatalytic system. This study enriches the application of photocatalysis using molecularly imprinted nanocomposite materials for treating complex pollutant mixtures in water.
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WATER RESEARCH
·
2022
·
IF 13.4
Jun Liang,Kexin Chen,Xiaoguang Duan,Ling Zhao,Hao Qiu,Xiaoyun Xu,Xinde Cao
The impacts of pH on purification efficiency can be phenomenal in advanced oxidation processes (AOPs), because solution pH affects persulfate (PS) activation processes. However, consensus has not been reached on the regimes of pH-regulated oxidation in persulfate-based AOPs (PS-AOPs). Particularly, the impacts of pH on carbon-catalyzed generation of radical and nonradical species remain unclear. In this work, we evaluated three typical carbonaceous materials including pyrolytic carbon (PC), activated carbon (AC), and carbon nanotube (CNT) to activate PS for sulfamethoxazole (SMX) degradation within a pH range from 4 to 9. The experiment revealed pH-dependent SMX removal in PC/PS, AC/PS, and CNT/PS, and the kinetics followed an order of pH 4 > pH 7 > pH 9. Solution pH simultaneously affected SMX adsorption and degradation, but the latter was more profound. Chemical quenching experiment, electrochemical measurement, kinetics calculation, and ATR-FTIR tests collectively revealed that high pH was not favorable for both radical and nonradical oxidation. In the PC/PS system, increased pH decreased the amount of phenolic –OH on PC surface, thereby restraining the generation of SO 4 •− and • OH due to the lack of electron donors. For AC/PS system, elevated pH hindered the interactions between AC and PS, thus suppressing the formation of surface-bound radicals. CNT/PS initiated an electron-transfer pathway, and increased pH reduced the oxidation potential of surface CNT-PS* complex, which was not favorable for nonradical oxidation of adsorbed pollutants. Therefore, outcomes of this work will advance the current knowledge on the intrinsic impacts of pH in PS-AOPs catalyzed by carbonaceous materials for wastewater purification.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Qingdong Qin,Yuancheng Dong,Taiping Yu,Yongfeng Zhang,Yan Xu,Jingjing Yang
The development of a heterogeneous catalyst for efficient activation of peroxymonosulfate (PMS) is still highly desired in metal-based advanced oxidation processes . In this study, nickel-cobalt-iron hybrid oxides (NiCoFe-HO) catalyst was fabricated via direct thermal decomposition of nickel-cobalt hexacyanoferrate to activate PMS for sulfamethoxazole (SMX) degradation. NiCoFe-HO presented a much greater catalytic performance in SMX degradation with PMS under neutral pH ( k = 0.079 min −1 ). The degradation rate of SMX with NiCoFe-HO was 2.3 and 3.0 times higher than that with nickel-iron hybrid oxides and cobalt-iron hybrid oxides, respectively. The synergistic effect among Ni, Co and Fe was experimentally verified to elucidate the superior catalytic activity. Sulfate radical and singlet oxygen were identified as the predominant reactive species in the current oxidation process. SMX degradation efficiency was gradually enhanced with the increase of catalyst dosage, PMS dosage and temperature but decreased with the increase of pH. In addition, NiCoFe-HO showed good stability and reusability. This study extends the design of hybrid metal oxides as efficient heterogeneous catalysts for PMS activation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Dong-Hua Xie,Pu-Can Guo,Keng-Qiang Zhong,Guo-Ping Sheng
A self-assembly strategy was presented for the synthesis of highly dispersed Co/Fe bimetallic carbon cages (CoFe50@C) through thermal morphology-controlled transformation of Fe doping dual metal-organic frameworks (MOFs). Taking advantage of the well dispersibility, synergetic effects between Fe and Co species, and enhanced graphitization degree of carbon, CoFe50@C exhibited a high removal efficiency of 98% in 180 min for sulfamethoxazole (SMX). The synergistic effect between Co and Fe species played an important role in promoting the reduction of Co(III) to Co(II) and the adsorption of H 2 O 2 molecules, thus enhancing the generation of hydroxyl radicals (HO•), which had been demonstrated by density functional theory (DFT) calculations. Meanwhile, the graphitized carbon cages could prevent the loss of bimetallic active component and promote the electron transfer during catalytic reaction . This work provides a new type of highly dispersed Co/Fe bimetal carbon cages as heterogeneous Fenton nanocatalyst for the degradation of organic contaminants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yinhao Dai,Chengdu Qi,Hui Cao,Yanni Wen,Yijie Zhao,Chenmin Xu,Shaogui Yang,Huan He
In this study, microwave (MW)-activated peracetic acid (PAA) system was used for the removal of sulfamethoxazole (SMX, a typical aquatic sulfonamide antibiotic). The rate constant of SMX degradation in the MW/PAA system was about 1.39 times of conventional heating activated PAA system. In MW/PAA system, alkaline condition was more favorable to the SMX degradation than neutral and acidic conditions. Different influencing factors, including the MW output power, reaction temperature, initial PAA concentration and common coexisting substances (Cl – , HCO 3 – and humic acid), on SMX degradation in MW/PAA system were systematically studied. The results showed that increasing the MW power, the reaction temperature or the concentration of PAA can promote the degradation of SMX. In addition, Cl – slightly promoted SMX degradation, while HCO 3 – and humic acid significantly inhibited the SMX degradation. The results of quenching and electron paramagnetic resonance experiments indicated that the reaction is dominated by a non-radical process, i.e., singlet oxygen ( 1 O 2 ), followed by radical processes of carbon-centric radicals (R–C • ). Based on the results of liquid chromatography-tandem mass spectrometry and theoretical calculations, four pathways of SMX degradation, including benzene ring hydroxylation, amino-oxidation, self-coupling and S-N bond breakage, were proposed. Toxicity of SMX and its intermediate products was predicted by the ECOSAR program, which indicated that SMX was converted to less toxic substances. This work provides theoretical implications for further development of the PAA-based advanced oxidation process for organic contaminants removal in water/wastewater.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 29
·44732-44745
·
IF 5.19
Wang Zhijie,Bao Jianguo,Du Jiangkun,Luo Liting,Xiao Guangfeng,Zhou Ting
Pollutant degradation via periodate ( \({\text{IO}}_{4}^{-}\) ) and transitional metal oxides provides an economical, energy-efficient way for chemical oxidation process in environmental remediation. However, catalytic activation of periodate by manganese dioxide and the associated mechanism were barely investigated. In this study, four MnO 2 polymorphs (α-, β-, γ- and δ-MnO 2 ) were synthesized and tested to activate \({\text{IO}}_{4}^{-}\) for the degradation of sulfamethoxazole (SMX). The reactivity of different MnO 2 structures followed the order of α-MnO 2 > β-MnO 2 > γ-MnO 2 > δ-MnO 2 , suggesting that the particular crystalline structure in α-MnO 2 would exhibit higher activities via \({\text{IO}}_{4}^{-}\) activation. Herein, in α-MnO 2 / \({\text{IO}}_{4}^{-}\) system, 91.1% of SMX was eliminated within 30 min with degradation rate constant of 0.0649 min −1 , and the neutral pH exhibited higher efficiency in SMX degradation compared with acidic and alkaline conditions. Singlet oxygen ( 1 O 2 ) was unveiled to be the dominant ROS according to the results of electron paramagnetic resonance, chemical probes and radical quenching experiments, whereas \({\mathrm{O}}_{2}^{\bullet -}\) and • OH were mainly acted as a free-radical precursor. Six oxidation products were identified by LC–MS, and the elimination of sulfonamide bond, hydroxylation and direct oxidation were found to be the important oxidation pathways. The study dedicates to the mechanistic study into periodate activation over alpha-MnO 2 and provides a novel catalytic activation for selective removal in aqueous contaminants.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Suxin Li,Yanbin Tong,Hongyu Dong,Jianjiang Lu,Junfeng Niu
The electrochemical degradation performance of sulfamethoxazole (SMX) was studied in the presence of humic acid (HA) by using a Ti/Ti 4 O 7 /β-PbO 2 anode. The electrochemical degradation efficiency of SMX decreased from 93.4% to 45.8% in 50 min after the addition of 25 mg L −1 HA. The pseudo-first-order kinetic rate constant decreased by 71.4%, and the E EO value increased from 63.8 Wh L −1 to 90.9 Wh L −1 . HA and its degradation intermediates could compete for free radicals, especially for ·OH, with SMX. The analytical results obtained using UPLC-ESI-Q-TOF-MS showed that 18 degradation intermediates were identified in the coexistence of SMX and HA. Four imine intermediates were formed through the reactions between the aniline moieties of SMX and quinone groups in the HA structure through covalent bonds . Furthermore, the relative abundances of the intermediates demonstrated that the imine intermediates were complex and stable during electrochemical degradation.
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