ENVIRONMENTAL RESEARCH
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2021
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IF 6.498
Peng He,Yao Xiong,Yaozong Chen,Mengfei Liu,Jianyu Zhu,Min Gan
Along with rapid development of sulfate radicals-based advanced oxidation process , efficient, alternatively eco-friendly and cost-effective catalyst is of uppermost priority. However, expensive chemicals are used as source of metal in most of these catalysts, and lose sight of the abundant natural mineral resources on immediate surroundings. In this work, montmorillonite and hematite, two of abundantly natural minerals were utilized to prepare a persulfate catalyst (TMH@M) for sulfamethoxazole (SMX) degradation. The results indicated more than 91% of SMX was removed within 60 min in TMH@M/PS system. The degradation efficiency of SMX of TMH@M/PS combined system was impacted by SMX concentration, PS dosage and natural organic matters, and can remain stable in a certain concentration of HA/chelating agent and a wide pH range (3.01–9.06). Radical scavenging and EPR tests demonstrated 1 O 2 , OH, and SO 4 - were major reactive oxygen species in the TMH@M/PS system, while the latter seems more important for degradation of SMX. The results of SEM-EDS, XRD and XPS conformed that low valence iron species (Fe 0 , Fe 2+ and Fe 3 O 4 ) on TMH@M surface are the main driving force behind PS activation to generate reactive species. Furthermore, the iron species on TMH@M surface were transformed during reaction, that in favor of mitigating metal leaching. This work presented a method based on ubiquitous natural minerals to prepare catalyst with excellent PS activate performance for organic wastewater treatment implying a new strategy in minerals utilization deeply and a promisingly alternative process for organic wastewater treatment based on mineral materials.
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高影响因子
MOLECULES
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2020
·Vol. 25
·期 12
·2725
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IF 3.267
Xuefei Zhou,Haowei Wu,Longlong Zhang,Bowen Liang,Xiaoqi Sun,Jiabin Chen
Advanced oxidation processes (AOPs) are effective ways to degrade refractory organic contaminants, relying on the generation of inorganic radicals (e.g.,•OH and SO4•−). Herein, a novel AOP with organic radicals (R-O•) was reported to degrade contaminants. Lanthanum cobaltite perovskite (LaCoO3) was used to activate peracetic acid (PAA) for organic radical generation to degrade sulfamethoxazole (SMX). The results show that LaCoO3exhibited an excellent performance on PAA activation and SMX degradation at neutral pH, with low cobalt leaching. Meanwhile, LaCoO3also showed an excellent reusability during PAA activation. In-depth investigation confirmed CH3C(O)O•and CH3C(O)OO•as the key reactive species for SMX degradation in LaCoO3/PAA system. The presence of Cl−(1–100 mM) slightly inhibited the degradation of SMX in the LaCoO3/PAA system, whereas the addition of HCO3−(0.1–1 mM) and humic aid (1–10 mg/L) could significantly inhibit SMX degradation. This work highlights the generation of organic radicals via the heterogeneous activation of PAA and thus provides a promising way to destruct contaminants in wastewater treatment.Keywords:advanced oxidation processes (AOPs);peracetic acid;LaCoO3;organic radicals
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ELECTROCHIMICA ACTA
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2025
·
IF 5.6
Hailun Zhao,Jian Ke,Shangkun Zhu,Manting Li,Jianqiu Chen,Qiulian Yang
The performance of Fe-catalyzed electrochemical advanced oxidation in antibiotic degradation was typically hampered by poor reduction efficiency of Fe 3+ to Fe 2+ and a narrow pH working range. This work employed natural hematite (HM) as iron source and oxalic acid (OA) as complexing agent in conjunction with electrolysis (EC) to address these concerns. Results showed that the EC/HM/OA system can achieve a 99.77 % degradation efficiency of sulfamethoxazole (SMX) under the optimized reaction conditions. The SMX degradation rate constant in EC/HM/OA system was 2.53-fold higher than in EC/HM system, following pseudo first-order kinetics. The OA addition promoted the Fe 3+ reduction by complexing with HM in electrochemical system, as well as extended the pH application range of EC/HM system to 3 − 11. The ATR−FTIR test and DFT calculation demonstrated that the adsorption of OA on the HM surface occurred in a deprotonated bidentate mononuclear configuration. Radical quenching experiments and EPR analysis confirmed that the crucial reactive oxygen species for SMX degradation in EC/HM/OA system were the ·OH and ·O 2 - radicals. Five potential degradation pathways of SMX were proposed. ECOSAR model and Daphnia magna toxicity tests demonstrated attenuated toxicity of SMX after degradation. The EC/HM/OA system exhibited robust resistance to common anions (Cl⁻ and NO₃⁻), and achieved high SMX degradation (86.82 %–99.67 %) across different water matrices. The combination of natural HM with OA significantly improved the degradation performance of electrochemical process for persistent antibiotics.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2018
·
IF 3.779
Chao Wang,Yao Xue,Peifang Wang,Yanhui Ao
It is necessary to find visible light responsive photocatalysts for rapid and simple degradation of organic pollutants in water environment. In this work, a visible light responsive composite photocatalyst AgI/UiO-66 was prepared by an in situ growth method. Sulfamethoxazole (SMZ) antibiotic was selected as the target contaminant to probe the photocatalytic performance of the as-prepared AgI/UiO-66 composite under visible light irradiation. The results showed that the photocatalytic performance of the AgI/UiO-66 composite enhanced significantly compared to pure AgI. The effects of typical environment factors (i.e. pH, inorganic salt ions and common anions) on the degradation of SMZ were evaluated extensively. Results showed that the investigated pH (5.2, 7.0, 9.5) had no apparent effect on the photocatalytic degradation of SMZ except pH 2.5, at which the degradation rate of SMZ decreased significantly. In addition, inorganic salt ions and Cl − , HCO 3 − and SO 4 2− anions in water exhibited no apparent effect on the degradation of SMZ. The effect of water matrix on the degradation of SMZ was also investigated. In the river water, the removal efficiency of SMZ was reduced compared with the cleaner water matrix. The capture experiments of radicals confirmed that superoxide radicals ( O 2 − ) and hydroxyl radicals ( OH) were the main active species for the photocatalytic degradation of SMZ in the present work. Finally, the tentative degradation pathways of SMZ were proposed based on the intermediates analysis.
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FOOD CHEMISTRY
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2020
·
IF 6.306
Long Li,Ying Zhu,Feiyu Zhang,Hui Li,Jibran Iqbal,Ting Wu,Yiping Du
In this work, in-syringe membrane solid-phase extraction (MSPE) device was fabricated for the on-site sampling of sulfamethoxazole (SMX) in food samples followed by solid-phase fluorescence spectra analysis. The samples and fluorescamine (FA) were added to a syringe for derivation. Then, the derivative of SMX was extracted by a membrane in the syringe SPE device. Subsequently, the derivative on the membrane was measured immediately without additional elution procedure. The method was successfully applied in plasma, milk, and egg samples for the trace SMX detection, with the recovery of 98%–102%, RSDs from 1% to 6%. Compared with liquid chromatography, direct detection of the concentrated analyte significantly improved the sensitivity. Moreover, fluorescamine made it unnecessary to separate SMX from the interference. Consequently, it was a time-saving, low-cost, and easy-operation method, which demonstrated the potential of in-syringe SPE as a promising candidate for on-site analysis.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Pin Peng,Xinyu Yan,Lixiang Chen,Xiang Li,Huiying Yang,Yijing Miao,Feng Zhao
Livestock wastewater is characterized by high concentrations of organic matter and diverse antibiotics. A major challenge in its anaerobic treatment is the effective degradation and thorough removal of coexisting antibiotic contaminants. In this study, an external voltage was applied to establish an electroactive biofilm, thereby enhancing the co-metabolic degradation of sulfamethoxazole and roxarsone. Application of +0.6 V (Ag/AgCl) increased the 72 h TOC removal efficiency to 52.1 %. At the same time, sulfamethoxazole and roxarsone removal efficiencies reached 90.8 % and 100 %, respectively. The results from liquid chromatography-mass spectrometry (HPLC-MS/MS) and density functional theory calculations revealed sulfamethoxazole degradation pathways: N–O bond cleavage and hydroxylation. Roxarsone degradation primarily involved nitro group reduction and C–As bond cleavage. The pharmacophore of sulfamethoxazole was effectively removed, and inorganic arsenic from roxarsone degradation was efficiently immobilized. Toxicity analysis confirmed that the electroactive biofilm notably reduced toxic intermediate accumulation. Elevated concentrations of NADH and ATP in the electroactive biofilm indicated enhanced microbial substrate metabolism and generation of more electron donors. The higher absolute abundance of the sulfamethoxazole degradation gene ( SadABC ) in the electroactive biofilm indicated that sulfamethoxazole degrading enzyme (sadABC) gained more electrons. Microbiome analysis revealed the upregulation of genes linked to extracellular electron transfer, the tricarboxylic acid (TCA) cycle, nitro-reduction, and sulfate reduction pathway, confirming the electroactive biofilm enhances substrate metabolism and co-metabolic antibiotic degradation. Electroactive biofilm offers a viable strategy for antibiotic removal in livestock wastewater.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2024
·
IF 6.2
Guanghua Xiong,Haiyan Zhang,Huangqi Shi,Yulin Peng,Meiling Han,Tianle Hu,Xinjun Liao,Yong Liu,Jun’e Zhang,Gaoxiao Xu
The combined pollution of microplastics (MPs) and sulfamethoxazole (SMZ) often occurs in aquatic ecosystems, posing a serious threat to animal and human health. However, little is known about the liver damage caused by the single or co-exposure of MPs and SMZ, and its specific mechanisms are still poorly understood. In this study, we investigated the effects of co-exposure to 20 μm or 80 nm MPs and SMZ in both larval and adult zebrafish models. Firstly, we observed a significant decrease in the number of hepatocytes and the liver damage in larval zebrafish worsened following co-exposure to SMZ and MPs. Additionally, the number of macrophages and neutrophils decreased, while the expression of inflammatory cytokines and antioxidant enzyme activities increased after co-exposure in larval zebrafish. Transcriptome analysis revealed significant changes in gene expression in the co-exposed groups, particularly in processes related to oxidation-reduction, inflammatory response, and the MAPK signaling pathway in the liver of adult zebrafish. Co-exposure of SMZ and MPs also promoted hepatocyte apoptosis and inhibited proliferation levels, which was associated with the translocation of Nrf2 from the cytoplasm to the nucleus and an increase in protein levels of Nrf2 and NF-kB p65 in the adult zebrafish. Furthermore, our pharmacological experiments demonstrated that inhibiting ROS and blocking the MAPK signaling pathway partially rescued the liver injury induced by co-exposure both in larval and adult zebrafish. In conclusion, our findings suggest that co-exposure to SMZ and MPs induces hepatic dysfunction through the ROS-mediated MAPK signaling pathway in zebrafish. This information provides novel insights into the potential environmental risk of MPs and hazardous pollutants co-existence in aquatic ecosystems.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Ying Ding,Jin-Ting Zheng,Shuai Du,Di Wu,Feng Hu,Dong Zhu
Microplastics (MPs) are currently receiving widespread attention worldwide, and their co-occurrence with antibiotics is unavoidable. However, our understanding of how protists respond to co-pollution and mediate antibiotic resistance genes (ARGs) profiles remains exceedingly limited, particularly within non-target animals’ guts. To bridge these gaps, we investigated the individual and combined effects of polyethylene and sulfamethoxazole (SMZ) on microbial communities and ARGs in soil and earthworm guts. We found that the MP–SMZ combination significantly elevated the abundance and richness of ARGs in the soil and earthworm. Protistan compositions (particularly consumers) responded more strongly to pollutants than did bacterial and fungal communities, especially under combined pollution. Interkingdom cooccurrence network analysis revealed that protists had stronger and more effective interactions with the resistome in the earthworm guts, suggesting that the impact of these protists on ARGs compositional changes was potentially modulated through the “top-down” regulation of bacteria and fungi. Meta-cooccurrence networks further confirmed that protist-related networks had more keystone pollution-sensitive ASVs ( ps ASVs) and these ps ASVs were mostly associated with protistan consumers. Our study highlights protists as promising agents for regulating and monitoring microbial functions, as well as the ecological risks of the antibiotic resistome associated with MPs and SMZ pollution in agricultural ecosystems.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xintao Fu,Yan Lin,Chunping Yang,Shaohua Wu,Yue Wang,Xiang Li
Transition-metal phosphides (TMPs) have been considered a promising candidate for heterogeneous catalysis in wastewater treatment , while the feasibility of its application in peroxymonosulfate (PMS) based advanced oxidation processes systems for the treatment of high-salinity organic wastewater remains still unclear. In this study, catalysts of cobalt phosphide (CoP) nanoparticles confined in nitrogen-doped porous carbon (CoP/NC) were prepared using zeolitic imidazolate framework-67 (ZIF-67) as a template via calcination-oxidation-phosphorization, which were subsequently applied to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX) in the water with high-salinity concentrations. Results showed that the degrading performance of CoP/NC could be improved and regulated by phosphorus (P) doping amount with an optimum of 5.0% (CoP/NC-5), which reached 100% of SMX degradation. Meanwhile, CoP/NC-5 catalyst could tolerate wide pH variations (5–9). More importantly, the CoP/NC-5/PMS system showed high adaptability to various concentrations of inorganic salt, even up to 500 mM. In addition, active species of sulfate radical (SO 4 •− ) and singlet oxygen ( 1 O 2 ) were identified, which played dominant roles in the destruction of SMX, and the production amount of SO 4 •− was quantified. This work confirmed that transition-metal phosphides nanoparticles confined in nitrogen-doped porous carbon were a promising catalyst for SMX elimination in high saline wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shizong Wang,Jianlong Wang
High efficient activator is highly desired in the field of persulfate-based advanced oxidation process. In comparison with the previous studies, this study adopted nitrogen, sulfur and oxygen co-doped carbon material to support Fe 0 encapsulate in Fe 3 O 4 to prepare iron-based modified carbon composite (Fe 0 @Fe 3 O 4 -MC) by a facile two-step pyrolysis. Fe 0 @Fe 3 O 4 -MC was then used for degradation of sulfamethoxazole. The results showed that Fe 0 @Fe 3 O 4 -MC had superior catalytic activity for PMS activation due to the synergistic effect of iron-based compound and modified carbon. In the presence of 0.1 g/L of Fe 0 @Fe 3 O 4 -MC, SMX (0.04 mM) could be completely degraded within 120 min at pH 3.4 and 3 mM of PMS. The SMX degradation followed pseudo first-order kinetic model, with the rate constant of 0.12 min −1 , and the mineralization of SMX achieved 48.4%. Sulfate radicals dominated in the SMX degradation. In addition to Fe 0 and Fe 3 O 4 , carbon defects, graphitic N, sulfur and FeN 4 also contributed to PMS activation. Fe 0 oxidation was the rate-limiting step for PMS activation. Dissolved oxygen made a minor contribution to Fe 0 oxidation. The intermediate products of SMX degradation were identified, and two pathways of SMX degradation were proposed. The influencing factors on SMX degradation were studied, including pH, temperature, PMS concentration, Fe 0 @Fe 3 O 4 -MC dosage, chloridion, carbonate and humic acids, and the influencing mechanism was discussed. This study could provide an efficient PMS activator for the degradation of emerging organic pollutants in water and wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Haiqiang Qi,Xiuping Sun,Zhirong Sun
Bifunctional electrodes have attracted significant research interest in the field of heterogeneous electro-Fenton (hetero-EF) process for efficient treatment of antibiotic-containing wastewater. In this study, etched graphite felt (EGF) was used as the matrix material because of its excellent electrochemical properties, rich pore structure, and large specific surface area. The transition metals Cu and Fe were in situ grown on the EGF electrode surface without polymer binder by a one-step hydrothermal method. The obtained electrode consisting of Cu-doped Fe 2 O 3 nanoparticles/EGF (Cu-Fe 2 O 3 /EGF) was used in the hetero-EF process for in situ electro-generation and activation of hydrogen peroxide (H 2 O 2 ) for efficient degradation of sulfamethoxazole (SMX). The Cu-Fe 2 O 3 /EGF electrode demonstrated a wide pH application range of 3.0–9.0. According to electron spin resonance and free-radical quenching experiments, hydroxyl radical and superoxide anion were the dominant species in the hetero-EF process, while the hydroxyl radical played a major role in the degradation of SMX. In consecutive runs, the electrode exhibited low metal ion leaching and excellent stability. Furthermore, the possible mechanism for the production and activation of H 2 O 2 as well as possible SMX degradation pathways were proposed. The toxicity of SMX samples during degradation exhibited a decreasing trend according to the results of toxicological simulation and Escherichia coli growth test. This study provides a new strategy for the construction of an efficient and stable bifunctional cathode for the advanced treatment of antibiotic-containing wastewater.
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EUROPEAN JOURNAL OF PHARMACEUTICAL SCIENCES
·
2021
·
IF 4.384
Ling-Yang Wang,Fan-Zhi Bu,Yue-Ming Yu,Yuan-Yuan Niu,Yan-Tuan Li,Cui-Wei Yan,Zhi-Yong Wu
In order to exploit the advantages to the full of multidrug salification strategy in amending the pharmaceutical properties of drugs both in vitro and in vivo , and further to open up a new way for its applications in bacteria-virus mixed cross-infection drugs, a novel dual-drug crystalline molecular salt hybridizing antibacterial drug sulfamethoxazole (SFM) with antiviral ingredient amantadine (ATE), namely SFM-ATE, is successfully designed and synthesized via multidrug salification strategy oriented by proton exchange reaction. The crystal structure of the firstly obtained molecular salt is precisely identified by employing single-crystal X-ray diffraction and multiple other techniques. The results show that, in the crystal lattice of molecular salt SFM-ATE, the classical hydrogen bonds together with charge-assisted hydrogen bonds contribute to two- dimensional networks, between which the hydrophobic interaction plays an important role. The relevant in vitro/vivo pharmaceutical properties of the dual-drug molecular salt are carried out through a comparative investigation of theoretical and experimental methods. It has been found that SFM displays concurrent improvements over the bulk drug in its permeability and dissolution after forming the molecular salt, which is supported by the molecular electrostatic potential calculation and Hirshfeld surface analysis. Encouragingly, the perfected in vitro biopharmaceutical properties can effectually turn into the in vivo pharmacokinetic preponderances with the expedited peak plasma concentration, lengthened half-life and enhanced bioavailability. Better yet, the antibacterial activities of SFM from the molecular salt get stronger with enlargement in inhibition areas and reduction in values of minimum inhibitory concentrations against the tested bacterial strains. Consequently, the present contribution not only supplies an opportunity for widening applications for classical sulfa drugs via dual-drug salification strategy, but also offers an alternative approach in dealing with viral-bacterial coinfection even other complex diseases by drugs’ hybridization at the molecular level.
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