CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yi Xie,Xuqian Wang,Wenhua Tong,Wanrong Hu,Panyu Li,Linli Dai,Yabo Wang,Yongkui Zhang
Fe-based phosphide has shown tremendous potential for heterogeneous catalysis due to its superior activity. Herein, a series of Fe x P/biochar composites were successfully prepared through a simple pyrolysis process. Iron species (FeOOH) was pre-loaded on the surface of phosphorus-containing biomass (yeast), which was subsequently converted to FexP/biochar with the assistance of in-situ produced reducing gases (H 2 , CO, PH 3 , etc.). When applied for typical antibiotic pollutant (sulfamethoxazole, SMX) removal, the optimal material (Fe x P/BC-5) performed well with a 99% removal efficiency in 30 min via the synergistic effects of adsorption and degradation by activation of dissolved oxygen (DO). Reactive oxygen species, including H 2 O 2 , ·OH, O 2 − and 1 O 2 , were generated in Fe x P/BC-5/DO system by charge transfer and Fenton-like reaction. Fe x P/BC-5 was applicable in a broad pH range from 3.0 to 9.0 and exhibited good reusability in five recycle runs after regeneration. Moreover, the primary reactions in SMX degradation process were discussed based on identified intermediates by liquid chromatography–mass spectrometry (LC–MS). This work not only develops a simple approach to construct iron phosphides/biochar using green and sustainable phosphorus source but also bring new insights for environmental pollutants remediation by oxygen activation.
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Journal of Ocean University of China
·
2020
·Vol. 19
·期 4
·865-873
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IF 0.802
Zheng Bingbing,Pang Wenhui,Zhao Yangguo,Guo Liang,Gao Mengchun,Jin Chunji,She Zonglian
The wide application of antibiotics in aquaculture requires an efficient treatment of the wastewater before discharging it into the environment. During the wastewater treatment, the influence of antibiotics on the performance of bioreactor should be well revealed due to their toxicity to the functional microbial community. In this study, the effect of feeding 10–30 mgL −1 sulfamethoxazole (SMX) in influent on the performance of an anoxic/oxic-moving bed biofilm reactor (A/O-MBBR) treating mariculture waste-water and the responding change of biofilm microbial communities was investigated. The COD average removal rate remained at 94.61%–97.34% with the dosage of SMX. Compared with that, the nitrifying removals of NH 4 + -N and NO 2 − -N were violently inhibited by 30 mgL −1 SMX and denitrifying removal of the NO 3 − -N decreased obviously with 20 mgL −1 or more SMX. The microbial community in the successful startup bioreactor was relatively abundant, while the diversity of microbial community decreased with the increase of feeding SMX. The salt-tolerant and SMX-resistant genera Arcobacter, Thiothrix, Desulfuromusa and Nitrosomonas were gradually enriched and finally played a vital role in converting COD and recycling nitrogen and sulfur. Hence, the present A/O-MBBR reactor with the salt-tolerant functional microbiota achieved efficient removal of pollutants in the presence of low concentration (e.g., 10 mg L −1 ) SMX.
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Journal of Environmental Chemical Engineering
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2020
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IF 4.3
Aijiao Zhou,Xumeng Wu,Wangwei Chen,Lei Liao,Pengchao Xie
Powdered activated carbon embedded chitosan-polyvinyl alcohol composite (PAC/CS/PVA) beads were designed via a simple method for the adsorptive removal of hydrophilic sulfamethoxazole (SMX) and hydrophobic bisphenol A (BPA) from water. The as-prepared hydrogel was characterized, and the adsorption performances were comprehensively investigated. The maximum adsorption capacities of SMX and BPA on the adsorbent are 9.1 mg g −1 and 64.6 mg g −1 , respectively. The optimal pH was around 4 for SMX and 2–9 for BPA, respectively. Higher adsorbent dosages benefited the removal efficiencies but lowered the adsorption capacities. Both temperature and ionic strength slightly affect the adsorption of SMX and BPA. Pseudo-second-order model can well describe the adsorption of SMX and BPA on the hydrogel through spontaneous and endothermic process. Langmuir isotherm model performed better than Freundlich model to fit the equilibrium data. The stable adsorption capacities of SMX and BPA after used the hydrogel for 5 cycles evidenced its excellent reusability. The high adsorption capacities (> 7 mg g −1 for SMX, > 50 mg g −1 for BPA) in the presence of typical water matrices including Cl − , SO 4 2− , Cu 2+ and humic acid further suggest the good application potential of the fabricated PAC/CS/PVA beads.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Jingwen Wang,Bin Xiong,Lei Miao,Songlin Wang,Pengchao Xie,Zongping Wang,Jun Ma
In this study, peracetic acid (PAA) is successfully activated by cobalt ferrite (CoFe 2 O 4 /PAA) to remove sulfamethoxazole (SMX). Increasing either PAA (25–200 μM) or CoFe 2 O 4 (25–200 mg/L) dose accelerated SMX degradation in the CoFe 2 O 4 /PAA system, and the best removal of SMX (87.3%) was acquired with 200 μM PAA and 0.1 g/L CoFe 2 O 4 at neutral condition. Addition of humic acid or HCO 3 – inhibited SMX removal, whereas Cl – had little impact. The redox cycle of ≡Co 3+ /≡Co 2+ on the CoFe 2 O 4 surface dominated PAA activation to produce organic radicals (R-O • ) including CH 3 C(O)O • and CH 3 C(O)OO • accounting for SMX degradation. Based on the density functional theory (DFT) calculation and identified oxidation products, SMX transformation pathway was proposed to be initiated by electron transfer reaction with R-O • . The insignificant variation of acute toxicity, the fine CoFe 2 O 4 stability and the good removal of some other micro-organic pollutants suggested the potential applicability of the CoFe 2 O 4 /PAA system in degrading micro-organic pollutants.
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BIORESOURCE TECHNOLOGY
·
2019
·
IF 6.669
Shengnan Li,Tao Hua,Chung-Shin Yuan,Baikun Li,Xuya Zhu,Fengxiang Li
s Sulfamethoxazole (SMX) is a general antibiotic that is frequently identified in wastewater and surface water. In this study, the degradation and metabolic pathway of SMX by bio-electro-Fenton systems equipped with a CNT/r-FeOOH cathode were investigated. When initial SMX = 25 mg/L, the removal efficiency of SMX reached 94.66% by the bio-electro-Fenton system. The concentrations of sul 1, sul 2, sul 3, sul A , intI 1 and 16S rRNA genes were examined in effluents. Four out of the six ARGs analysed were detected. Among all quantified sul genes, sul 1 and sul A were the most abundant. High-throughput sequencing revealed that the microbial communities and relative abundance at the phylum and genus levels were affected by different SMX concentrations. In addition, the intermediates were detected and the possible SMX degradation pathway by the bio-electro-Fenton process in the present system was proposed. Furthermore, the highest power density obtained was 283.32 ± 16.35 mW/m 2 (SMX = 25 mg/L). This study provides an efficient and cost effective method for degrading antibiotics.
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CHEMOSPHERE
·
2019
·
IF 5.108
Juntao Tang,Jianlong Wang
Iron and copper bimetallic MOF material (Fe x Cu 1-x (BDC)) as a novel Fenton-like catalyst was prepared by a simple solvothermal method, and its performances were evaluated in the catalytic degradation of sulfamethoxazole (SMX) in the presence of hydrogen peroxide. The results indicated that the Fe x Cu 1-x (BDC)/H 2 O 2 system was highly effective for SMX degradation over a wide pH range (4.0–8.6). At initial solution pH of 5.6, the bimetallic Fe 0.75 Cu 0.25 (BDC) catalyst exhibited a 100% SMX (20 mg L −1 ) removal within 120 min, which was superior to the SMX removal efficiency over monometallic Fe(BDC) and Cu(BDC) catalysts. Combined with the physical-chemical characterization, the synergistic effect between Fe and Cu species were responsible for the efficient catalytic activity . Moreover, the Fe 0.75 Cu 0.25 (BDC) catalyst showed good reusability for SMX degradation. The possible reaction mechanism in Fe x Cu 1-x (BDC)/H 2 O 2 system was also tentatively proposed. This work has not only suggested the potential of bimetallic Fe x Cu 1-x (BDC) catalysts in Fenton-like treatment of antibiotics, but also provided useful information to develop MOF-based catalysts for efficient environmental remediation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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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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Journal of Environmental Chemical Engineering
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2023
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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
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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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APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Peng He,Chunyao Gu,Mengfei Liu,Jiancheng Chen,Junwen Chen,Junwu Liu,Yingchun Fang,Haijiao Xie,Jianyu Zhu,Min Gan
The treatment of emerging pollutants has become a challenging and multidisciplinary subject. Advanced oxidation processes based on persulfate are a strategic opportunity to address this issue, with research into catalysts and catalytic processes being the focus of this process. In this work, flower-like cobalt sulfide (F-CoS) particles acted as catalysts in peroxymonosulfate (PMS) activation for degrading an organic pollutant, sulfamethoxazole (SMX). The results indicated that F-CoS/PMS combined system performed excellently, with SMX being completely oxidized within 10 min. And the system exhibited superior resistance to environmental factors (e.g. pH and anions). Radicals quenching and electron paramagnetic resonance (EPR) analyses indicated that non-radical pathways based on high-valent cobalt-oxo (Co(IV)) species and 1 O 2 take a dominant position in SMX degradation, instead of SO 4 •− and •OH. Electrochemical, in-situ Raman and density functional theory (DFT) calculations revealed that PMS interacts with Co sites on the F-CoS surface, and then electronic transfer processes occurred, in which PMS acts as an electron acceptor to produce Co(IV) species and as an electron donor to produce 1 O 2 . This study not only implies a method with great potential application in organic wastewater treatment but also contributes to further comprehending the heterogeneous activation process and catalytic mechanism of PMS.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 21
·60704-60716
·
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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