WATER SCIENCE AND TECHNOLOGY
·
2023
·Vol. 87
·期 5
·1202-1213
·
IF 2.7
Liu Zhenzhong,Wu Yang,Wan Siwen,Wang Boyan,Ji Hongliang,Xiang Xiaofang
View large Download slide View large Download slide Close modal Compared with the common synthesis methods of metal-organic frameworks (MOFs), Co/Cu-based bi-MOFs composite catalyst Co X Cu (10− X ) -MOFs ( X = 2, 4, 6, and 8) was prepared by a facile synthesis method at room temperature. The bi-MOFs composite catalyst was characterized by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD). The removal ability of sulfamethoxazole (SMX) by different Co:Cu rate bi-MOFs composite catalysts, single Co-based MOFs (zeolitic imidazolate framework-67, ZIF-67), and Cu-based MOFs (Hong Kong University of Science and Technology-1, HKUST-1) were investigated and the effects of peracetic acid (PAA) concentration, catalyst dosage, the common interfering substances (Cl − , HCO 3 − , SO 4 2− , HA) in water, and SMX removal were investigated. Through the analysis of different free radical scavengers and the changes of surface elements before and after the reaction, the oxidation mechanism was further explored, and the stability of Co 4 Cu 6 -MOFs was explored through repeated recycling. The experimental results demonstrate that Co 4 Cu 6 -MOFs have a high catalytic activity for PAA. Co 4 Cu 6 -MOFs/PAA show the best removal effect of SMX under neutral conditions and the presence of Cl − and HCO 3 - can promote the removal of SMX. Co 4 Cu 6 -MOF composites were synthesized and used for SMX removal. Application of PAA activation catalyst to generate R–O• for SMX removal. The effects of different environmental factors on the removal of SMX were discussed.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaohui Liu,Jiamin Xu,Ying Liu,Xuan Zhang,Shaoyong Lu,Bin Zhao,Xiaochun Guo,Jian Zhang,Beidou Xi,Fengchang Wu
Pollution of sulfamethoxazole (SMX) in rural domestic sewage are a great challenge for ecological security because of limited treatment. In this study, an electrolysis-integrated bio-rack constructed wetland system (EC-CW-P) without substrates was developed for enhancing SMX removal in rural domestic sewage. The dynamic performance and mechanism of SMX (1 mg L -1 ) removal, occurrence of antibiotic resistance genes (ARGs) and microbial community composition at 4 ~ 24℃ were assessed. Meanwhile, the simultaneous removal performance of phosphorus in EC-CW-P was also analyzed due to key role of substrate adsorption and iron flocculation. The results revealed that the removal efficiency of SMX could reach 97.13% at 4 ~ 24℃ in the EC-CW-P by the electrocatalysis and adsorption of a ferric iron coagulant and biodegradation. Moreover, efficient removal of 74.12%~99.52% total phosphorus (TP) was obtained through electrocoagulation because of the formation of ferric ions. The occurrence of SMX had no effect on TP removal because of the different removal pathway. It should be emphasized that the removal efficiency of SMX owing to high microbial and plant activity which may be due to the formation of iron film and micro current stimulation and TP owing to adsorption of iron mud remained high (>80%) when the electrode was gradually passivated. Overall, the performance of bio-rack CW system was intensified by electrolysis (iron electrode) with higher bacterial abundance and plant activity in the EC-CW-P. However, the high relative abundance of sul ARGs (from 2.15 × 10 -1 to 2.41 × 10 1 copies 16S rRNA -1 ) in the influent of the EC-CW-P may pose a severe threat to ecosystem. These results provide a novel perspective for enhancing SMX and phosphorus removal by bio-rack constructed wetland system.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shuilian Cheng,Zhan Cen,Chengyang Tang,Li Xu,Zuofang Yao,Xiaosong Zhou,Qingyou Liu,Shengsen Zhang
Sulfamethoxazole (SMX), as a typical and widely-used antibiotic, its residue in the water environment poses a serious threat to human health and ecological balance. Herein, an environmentally friendly and cost-effective melamine sponge (MS) was utilized as a carrier for the preparation of three-dimensional (3D) porous cobalt and nitrogen co-doped carbon catalysts (Co-N/C) via an impregnation-pyrolysis method. This approach successfully yielded an easily recoverable Co-N/C@MS catalyst. By utilizing this catalyst to activate peroxymonosulfate (PMS), efficient degradation and purification of wastewater containing SMX were achieved. The experimental results showed that the Co-N/C@MS/PMS system achieved 98.39 % degradation efficiency, attributed to the sponge substrate's high pore structure allowing uniform catalyst dispersion. After four cycles, the system remained stable, addressing traditional powder catalysts' recovery and loss issues. Mechanistic studies revealed that C O, pyrrolic N, and Co 2 + are the primary active sites in Co-N/C@MS for PMS activation. Both radical (primarily SO 4 ·- ) and non-radical (mainly 1 O 2 ) pathways contribute to SMX degradation, with the latter pathways playing a dominant role. The optimal design and performance evaluation conducted in this study offer a novel perspective on the application of recyclable flake catalyst materials for persulfate purification of organic wastewater.
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RSC Advances
·
2020
·Vol. 10
·期 3
·1595-1602
·
IF 3.119
Wei Zheng,Yawei Shi,Guozhu Liu,Bin Zhao,Liang Wang
Using organic salts as precursors, heteroatom-doped porous carbons prepared by in situ activation had surface areas of up to 2703 m2 g−1. These porous carbons have been found to be effective adsorbents for adsorption of sulfamethoxazole (SMX) from water. The effects of precursor type, calcination temperature, pH and ionic strength as well as the regeneration properties were investigated. The different adsorption performances of porous carbons were related to their textural structures and chemical properties, and a reasonable adsorption mechanism was proposed. The effects of different heteroatom functional groups on the adsorption of SMX were also analyzed in detail. For potential practical applications, the performance of the porous carbon for removing SMX from real water was also tested.
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PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Mengyuan Qi,Xiaodan Ma,Bin Liang,Liying Zhang,Deyong Kong,Zhiling Li,Aijie Wang
Sulfonamide antibiotics (SAs) have been produced and consumed on a large scale over the last few decades. SAs are a typical class of refractory contaminants that are omnipresent in various environments. Although several [phenyl]-SA-degrading bacteria and their corresponding genomes have been documented, limited genetic information is available for the degraders of heterocyclic products (e.g., 3-amino-5-methylisoxazole [3A5MI] produced via sulfamethoxazole [SMX] catabolism). In this study, the previously isolated SMX-mineralizing bacterial partners, Paenarthrobacter sp. P27 (responsible for the initial cleavage of the -C-S-N- bond of SMX and further degradation of [phenyl]-SMX) and Norcardiodes sp. N27 (responsible for 3A5MI catabolism), were further studied and their complete genomes were sequenced. Complete degradation and bacterial growth were verified by pure-culture experiments with SMX or 3A5MI as the sole carbon, nitrogen, and energy source. By cross-feeding strains P27 and N27, complete catabolism of SMX could be achieved over a wide range of initial SMX concentrations. Moreover, strain P27 was capable of transforming the additional nine SA representatives into their corresponding nitrogen-containing heterocyclic products, strongly indicating the broad substrate spectrum and marked bioremediation potential of strain P27. The genome of strain P27 contained the highly homologous monooxygenase gene cluster, sadABC , which initially attacked the sulfonamide molecules. The complete genome sequences of the two important degraders will benefit future research centering on the molecular mechanism underlying advanced SMX mineralization and will aid in further understanding the interspecific interactions and metabolite exchanges for the optimization of artificially constructed synthetic functional microbiomes.
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Jiali Peng,Peng Zhou,Hongyu Zhou,Wen Liu,Heng Zhang,Chenying Zhou,Leiduo Lai,Zhimin Ao,Shijun Su,Bo Lai
Many reagents as electron sacrificers have been recently investigated to induce decomposition of permanganate (KMnO4) to produce highly reactive intermediate Mn species toward oxidation of organic contaminants; however, this strategy meanwhile causes low KMnO4 utilization efficiency. This study surprisingly found that graphite can mediate direct electron transfer from organics (e.g., sulfamethoxazole (SMX)) to KMnO4, resulting in high KMnO4 utilization efficiency, rather than reductive sites of graphite-induced conversion of KMnO4 to highly reactive intermediate Mn species. The galvanic oxidation process (GOP) and comparative experiments of different organic contaminants prove that the KMnO4/graphite system mainly extracts electrons from organic contaminants via a one-electron pathway instead of a two-electron pathway. More importantly, the KMnO4/graphite system has superior reusability, graphite can keep a long-lasting reactivity, and the KMnO4 utilization efficiency elevates significantly after each cycle of graphite. The transformation of SMX in the KMnO4/graphite system mainly includes self-coupling, hydroxylation, oxidation, and hydrolytic reaction. The work will improve insights into the electron-transfer mechanism and unveil the advantages of efficient KMnO4 utilization in the KMnO4-based technologies in environmental remediation.
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 27
·27712-27725
·
IF 2.914
Zhuan Run,Wang Jianlong
Antibiotics are becoming ubiquitous emerging contaminants in the aquatic environments due to their large amount of production and extensive application, which have received increasing public concern. In this paper, the degradation and mineralization of sulfamethoxazole (SMX) by ionizing radiation in the presence of Fe 3 O 4 as Fenton-like catalyst were evaluated, the influencing factors, such as the initial SMX concentration, initial pH, water matrix, and radical scavenger, etc. were examined. The results demonstrated that SMX could be efficiently degraded. The addition of Fe 3 O 4 could improve the degradation efficiency of SMX and increased the dose constant at various SMX initial concentrations. More than 98% of SMX was degraded in Fe 3 O 4 /gamma radiation system at a wide range of pH (about 3.0–11.0). The mineralization of SMX in the presence of Fe 3 O 4 was increased by 200%. Adding free radical scavenger (tert-butyl alcohol) inhibited the degradation of SMX. The addition of Fe 3 O 4 enhanced the dose constant of ·OH, indicating that Fe 3 O 4 promoted the formation of hydroxyl radicals (·OH) and then improved SMX degradation and mineralization. The degradation efficiency of SMX in secondary effluent of WWTP decreased from 100 to 84% in secondary effluent compared with that in deionized water. The intermediate products during the degradation of SMX by ionizing radiation were identified by high-performance liquid chromatography, and a possible pathway of SMX degradation in such a system was tentatively proposed.
Schema illustration of SMX degradation by irradiation in the presence of Fe 3 O 4
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Biochar
·
2022
·Vol. 4
·期 1
·1-11
·
IF 11.452
Li Yinxue,Shang Hongru,Cao Yongna,Yang Chunhui,Feng Yujie,Yu Yanling
To remove antibiotics from waste water, an alkali active porous biochar, 850BC, was prepared from corncob xylose residue. In preparation, NaOH dipping was used for silicon removal and KOH activation was operated at 850℃. Further characterization containing BET, SEM, and FTIR were confirmed. 850BC possessed a huge specific surface area of 3043 m 2 ·g −1 , developed pore structure and abundant oxygen functional groups. The adsorption performance of sulfamethoxazole on 850BC was quick and efficient, and the adsorption capacity reached 1429 mg·g −1 , which was significantly higher than other adsorbents reported previously. While pseudo-second-order kinetic model and Langmuir model could better describe the adsorption, chemisorption dominated the SMX adsorption onto 850BC. In virtue of pore-filling and π–π interaction as major mechanism, a large surface area and rich oxygen-containing functional groups led to an excellent adsorption performance. Thus, this preparation method provided a biochar-based adsorbent with enhanced specific surface for efficient removal of antibiotic pollutants. Graphical Abstract
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Ruonan Guo,Yangyang Wang,Junjing Li,Xiuwen Cheng,Dionysios D. Dionysiou
In this study, the application potential of a nanohybrid MnO 2 incorporating Fe 2 O 3 (MF) as a peroxymonosulfate (PMS) activator was demonstrated under visible light irradiation. Due to the optical band structure of MF, electron dense regions could be formed by introducing Fe 2 O 3 nanoparticles via photogenerated carriers migration. The PMS activation performance coupled with visible light photocatalysis was evaluated to remove various organic pollutants in water, specifically sulfamethoxazole, sulfacetamide, carbamazepine, malachite green, tartrazine, rhodamine B, and 4-chlorophenol, accordingly, 90.0 %, 91.5 %, 87.6 %, 93.1 %, 97.1 %, 100 %, and 94.8 % of degradation efficiencies were achieved. Besides, the initial pH and co-existing inorganic ions at diverse concentrations did not significantly affect the degradation efficiency. More important, the sulfamethoxazole degradation pathway and reaction mechanism of the MF/PMS/Vis system were proposed. Therefore, this work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Zhongshuo Xu,Yanfan Jiang,Wei Huang,Yuhui Wang,Xinshan Song
Sulfamethoxazole (SMX) is prevalent as one of the most frequently detected antibiotics in rivers worldwide, and is listed as one of the priority antibiotics in China based on the persistence, bioaccumulation, toxicity and resistance. Recently, the effect of SMX on aerobic granular sludge has attracted increasing interest. However, how SMX influences the biodegradable polymer supported denitrifying granular sludge is still obscure. Herein, two groups with or without exposure to 1 mg/L SMX with initial nitrate concentrations of 15, 30, and 50 mg/L were constructed. Results showed that there was a negligible difference on nitrate removal efficiencies between two groups under stable period (all exceeded 95 %) in batch bioreactors with an HRT of 24 h, supported by an insignificance difference ( p > 0.05). However, the decline in the first-order decay kinetic constants of nitrate removal rate, NAR and NIR activities verified a slight inhibition of SMX on denitrification. Meanwhile, SMX also had an impact on the chemical and microbial properties on granular sludge. SMX boosted the EPS secretion with more humic acid, a delicate rise in PN/PS ratios and a decrease in zeta potential of EPS all favored the microbes' survival under SMX stress. SMX shifted the microbial compositions, namely, the microbes directly involving in PHBV degradation ( Caldimonas , denitrificans Comamonas / Diaphorobacter ) were enriched instead of some denitrifying microorganism that could not directly utilize PHBV ( Denitratisoma , Azospira ). Additionally, even though sul1 and sul2 were enriched, which was not readily accessible to receiving waters due to a good settling properties of granular sludge. This work contributes to a deeper understanding of the impact of SMX on this system, and is of great significance for the operation of granular sludge system for nitrate removal under antibiotic's stress.
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Catalysts
·
2025
·Vol. 15
·期 9
·854
·
IF 4
Han Cui,Qiwei Zhang,Shan Qiu
By modulating the mass ratio of hydrothermal agents to cobalt/iron precursors, Co3O4nanowires were successfully integrated into spinel-type Co/Fe@NF, forming a heterojunction anode for alkaline water electrolysis (AWE) hydrogen production. This Co3O4nanowire-assembled CoFe2O4nanosheet anode (Co/Fe(5:1)@NF) exhibits exceptional electrochemical oxygen evolution reaction (OER) performance, requiring only 221 mV overpotential to achieve 10 mA cm−2. Sulfamethoxazole (SMX) was employed as a model pollutant to investigate the anode sacrificial material; it achieved approximately 95% SMX degradation efficiency, reducing the OER potential of 50 mV/10 mA cm−2. SMX oxidation coupled with Co/Fe heterojunction structure partially substitutes the OER. Co/Fe heterojunction generates an internal magnetic field, which induces the formation of novel active species within the system. ·O2−is the newly formed active oxygen species, which enhanced the proportion of indirect SMX oxidation. Quantitative analysis reveals that superoxide radical-mediated indirect oxidation of SMX accounts for approximately 38.5%, Fe(VI) for 9.4%, other active species for 6.1%, and direct oxidation for 46.0%. The nanowire–nanosheet assembly stabilizes a high-spin configuration on the catalyst surface, redirecting oxygen intermediate pathways toward triplet oxygen (3O2) generation. Subsequent electron transfer from nanowire tips facilitates rapid3O2reduction, forming superoxide radicals (·O2−). This study effectively driven by indirect oxidation, with cathodic hydrogen production, providing a novel strategy for utilizing renewable electricity and reducing OER while offering insights into the design of Co/Fe-based catalyst.
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高影响因子
JOURNAL OF SOILS AND SEDIMENTS
·
2024
·Vol. 24
·期 4
·1639-1651
·
IF 2.8
Liu Zengyu,Chen Yuyun,Zhang Junqin,Wang Fei,Zhang Hongli,Yun Rongrong,Li Ling,Chilouch Chayma
Purpose The contamination of soil with antibiotics has become a hot issue for the environment and global public health. However, there are scarcely any studies on the occurrence forms of antibiotics in saline soil. Occurrence forms of antibiotics are related to bioavailability. Therefore, this study facilitates the evaluation of the ecological risk of antibiotics in saline soil. Materials and methods An experiment with artificial antibiotic contamination of soil and salinization simulations was conducted. The changes in the occurrence forms of oxytetracycline (OTC) and sulfamethoxazole (SMX) in saline soil were analyzed by continuous ultrasonic extraction. The factors for occurrence forms, including aging time and particle size fraction, were considered. Results and discussion Soil salinization promoted the conversion of OTC and SMX from acid-soluble and bound states to water-soluble and locked states. Oxytetracycline in saline soil was predominantly in the water-soluble and acid-soluble states, accounting for 54.9–83.7% of the total. Sulfamethoxazole as well is accounting for 66.1–82.1%. In addition, the aging process from 7 to 63 days facilitated the conversion of OTC and SMX from the water-soluble, acid-soluble, and bound states to the non-extractable locked states, resulting in reduced bioavailability. Since the content of extractable forms of OTC and SMX in saline clay was high, it favors conversion to a locked state. Conclusions Oxytetracycline and sulfamethoxazole in saline soil were mainly in bioavailable states. The aging effect reduced the bioavailability of OTC and SMX in saline soil. Clay had the low proportion of OTC and SMX in the bioavailable state, reducing environmental risks.
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