Téo Ferreux, Geoffroy Duporté, Linda Luquot, Julie Mendret, Elena Gomez, Stephan Brosillon
{"title":"Abatement of micropollutants and formation of transformation products in municipal wastewater effluent during ozonation: Complementarity of targeted and non-targeted analyses.","authors":"Téo Ferreux, Geoffroy Duporté, Linda Luquot, Julie Mendret, Elena Gomez, Stephan Brosillon","doi":"10.1016/j.jhazmat.2025.139426","DOIUrl":"10.1016/j.jhazmat.2025.139426","url":null,"abstract":"<p><p>A comprehensive approach combining target analysis, non-target screening, and suspect screening was employed to assess the effectiveness of ozonation in removing micropollutants at their native concentrations from wastewater effluent, using HPLC-HRMS. Eight pharmaceutical micropollutants were monitored during the wastewater ozonation to evaluate their removal efficiency at different ozone doses. A specific transferred ozone dose of 1.10 g<sub>O3</sub>.g<sub>C</sub><sup>-1</sup> was sufficient to eliminate over 90 % of seven of the compounds. Non-target screening revealed that the greatest number of ozonation transformation products formed at a low ozone dose of approximately 0.52 g<sub>O3</sub>.g<sub>C</sub><sup>-1</sup>. Increasing the ozone dose led to further degradation of these transformation products. Suspect screening identified 15 OTPs with confidence levels of 3 or higher. The formation kinetics of these compounds were assessed based on their chromatographic peak areas. Primary transformation products from highly ozone-reactive compounds were most abundant at lower ozone doses, whereas those derived from less reactive compounds formed at higher ozone doses. The integration of multiple analytical approaches highlighted both the effectiveness of ozonation for micropollutant removal at economically sustainable doses and the importance of better understanding and monitoring ozonation transformation products during ozonation and in subsequent treatment processes.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"496 ","pages":"139426"},"PeriodicalIF":11.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144791128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenyi Huang, Runzhe Zhang, Guoqiang Jiang, Lidan Xie, Yi Liu, Xinyi Lu, Zhikui Zhou, Yanyan Xia, Jian Wang, Xiaoyun Fan
{"title":"Formation of environmentally persistent free radicals (EPFRs) and electron transfer in conjugated polymers and alkane polymers during aging.","authors":"Wenyi Huang, Runzhe Zhang, Guoqiang Jiang, Lidan Xie, Yi Liu, Xinyi Lu, Zhikui Zhou, Yanyan Xia, Jian Wang, Xiaoyun Fan","doi":"10.1016/j.jhazmat.2025.139418","DOIUrl":"10.1016/j.jhazmat.2025.139418","url":null,"abstract":"<p><p>The electrons in environmental persistent free radicals (EPFRs) of aged microplastics (MPs) are highly mobile and reactive, readily interacting with oxygen and water to generate reactive oxygen species, possessing ecological hazards. However, it is still a big challenge to detect the formation of EPFRs and electrons in real-time by using the conventional technologies. Interestingly, the conductive atomic force microscopy (CAFM) can capture local electrical information on the sample surface with high resolution. Based on this, the present work provided an intuitive understanding of the dynamic evolution of surface currents in aged conjugated aromatic ring MPs and alkane chain MPs. The study found that photoexcitation induced electron transitions, promoting interactions between electrons and the chemical bonds of the polymers and ultimately generation of the persistent free radicals. Conjugated structures played a crucial role in the facilitating of electron transfer. And the aged PET MPs primarily generated carbon-centered and oxygen-centered free radicals, while the aged PS and PP MPs mainly produced oxygen-centered free radicals. Ultimately, the free electrons generated by the aged MPs enhanced their removal capacity for cationic dyes. This study provides a novel testing method and perspective to deeply investigate the formation of electrons on the surfaces of aged MPs.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"496 ","pages":"139418"},"PeriodicalIF":11.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144777422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ping Ge, Na Liu, Yeyao Wang, John P Giesy, Xiaowei Jin
{"title":"Isomer-specific ecotoxicity and occurrence of ibuprofen: Underestimated risks in aquatic ecosystems.","authors":"Ping Ge, Na Liu, Yeyao Wang, John P Giesy, Xiaowei Jin","doi":"10.1016/j.jhazmat.2025.139430","DOIUrl":"10.1016/j.jhazmat.2025.139430","url":null,"abstract":"<p><p>Ibuprofen (IBU) is used as a racemic mixture despite enantiomeric pharmacological differences. However, its stereoselectivity in aquatic ecosystems remains inadequately characterized, leading to potential environmental risk uncertainties. This study presents a comprehensive, integrated, multi-tiered evaluation of the enantioselective ecotoxicity, environmental fate, and ecological risk of IBU in aquatic environments. Chronic toxicity tests with D. magna and recombinant yeast nuclear receptor assays demonstrated significant enantio-selective effects, with S-IBU exhibiting as much as 8-fold greater toxic potency than R-IBU at environmentally relevant concentrations. Using chiral-specific toxicity data from our experiments and the literature, the predicted no-effect concentration (PNEC) for S-IBU was significantly less than those for racemic IBU and R-IBU. Environmental monitoring across the Wenyu River basin revealed prevalent IBU contamination with a detection rate of 96.8 % and maximum concentration of 431.7 ng/L, with predominance of S-IBU with an enantiomeric fraction of 0.57-1.0 in surface waters and wastewater treatment plant effluents. Ecological risk assessment indicated that IBU posed moderate to great risks to aquatic ecosystems, with 93.5 % of sites exceeding PNEC. These findings demonstrate that conventional risk assessments using only racemic IBU substantially underestimate ecological hazards. This highlights the necessity for enantioselective toxicity assessment and monitoring in chiral chemicals risk management.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"496 ","pages":"139430"},"PeriodicalIF":11.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144791132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A comprehensive review of contents, toxic effects, metabolisms, and environmental behaviors of brominated and organophosphorus flame retardants.","authors":"Tuantuan Fan, Zhenfei Yan, Wenjie Huang, Weiying Feng, Yingchen Bai, Chenglian Feng, Fengchang Wu","doi":"10.1016/j.jhazmat.2025.139428","DOIUrl":"10.1016/j.jhazmat.2025.139428","url":null,"abstract":"<p><p>As emerging contaminants, flame retardants are ubiquitous in water, soil, the atmosphere, and organisms. Brominated (BFRs) and organophosphorus flame retardants (OPFRs) dominate as primary replacements for brominated diphenyl ethers, yet their comparative ecotoxicity and environmental behavior remain critically understudied. This study comprehensively summarizes environmental levels, toxicities, metabolism, and environmental behaviors between BFRs and OPFRs. It is showed that OPFRs have surpassed BFRs by 1 - 2 orders of magnitude in concentration becoming dominant contaminants across environmental matrices. OPFRs exhibit similar toxicity targets yet more complex metabolic pathways than BFRs, indicating that they are not environmentally safer alternatives. Meanwhile, they undergo microbial degradation as carbon substrates, photolysis as photosensitizers, and hydrophobic adsorption onto organic matrices (e.g., dissolved organic matter). These environmental behaviors may enhance or inhibit toxicity risk of flame retardants. In addition, the removal technologies and regulatory measures for flame retardants still require continuous refinement. Future studies should prioritize combined risk assessment of mixtures especially metabolites, environmental behaviors, and identification of the key environmental factors of flame retardants.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"496 ","pages":"139428"},"PeriodicalIF":11.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144796531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wei Li, Si-Xue He, Yi-Wen Liu, Qian-Yu Zhou, Shu-Fen Xiao, Yanshan Chen, Yue Cao, Lena Q Ma
{"title":"Arsenite antiporters ACR3/3;1 are critical for Se-enhanced plant growth and As accumulation in As-hyperaccumulators Pteris multifida and Pteris cretica.","authors":"Wei Li, Si-Xue He, Yi-Wen Liu, Qian-Yu Zhou, Shu-Fen Xiao, Yanshan Chen, Yue Cao, Lena Q Ma","doi":"10.1016/j.jhazmat.2025.139434","DOIUrl":"10.1016/j.jhazmat.2025.139434","url":null,"abstract":"<p><p>Selenium (Se) enhances plant growth and As accumulation in As-hyperaccumulator Pteris vittata, but its effects on As-hyperaccumulators Pteris multifida and Pteris cretica are unknown. Here, they were exposed to 50 μM arsenate (As<sub>50</sub>) plus 1.25 (Se<sub>1.25</sub>) or 2.5 μM (Se<sub>2.5</sub>) selenate under hydroponics. After 2 weeks of growth, the biomass, As, Se and malondialdehyde (MDA) contents, and important genes related to As metabolism in two plants were determined. Both plants were able to take up and translocate As to the fronds, with Se-enhanced plant growth being observed only under As exposure. For both plants, the As+Se treatments increased their biomass by 22-32 % compared to the As<sub>50</sub> treatment, which may be attributed to 42-45 % reduction in the MDA contents. However, the effects of Se on plant growth and As accumulation varied with Se doses and plant species. For P. multifida, 1.25 µM Se enhanced the As content by 52 % to 329 mg kg<sup>-1</sup> in the fronds, while 2.5 µM Se decreased. For P. cretica, Se promoted its frond As contents by 42-106 % to 155-225 mg kg<sup>-1</sup>, with 2.5 μM being more effective. Though showing little effect on phosphate transporter Pht1 or arsenate reductase HAC1, Se induced upregulation of arsenite antiporters ACR3/3;1 by 1.6-3.0 fold, which promoted As translocation from the roots to fronds and As sequestration into the fronds under As exposure. Se effectively enhances plant growth and As accumulation in P. multifida and P. cretica by upregulating the expression of arsenite antiporters ACR3. Based on literature and our data, ACR3/3;1 play critical roles in Se-enhanced As accumulation in As-hyperaccumulators, which may have application in phytoremediation of As-contaminated soils in temperate zones.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"496 ","pages":"139434"},"PeriodicalIF":11.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144801371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Luwei Li, Xuecong Qian, Shilong Wang, Yun Liu, Da Wang, Huixin Zhang, Yechen An, Haijun Cheng, Jun Ma
{"title":"Unveiling non-radical oxidation pathways in peroxymonosulfate/cobalt(II) systems: Critical role of cobalt(III) and cobalt(IV) explored by manganese(II) probing.","authors":"Luwei Li, Xuecong Qian, Shilong Wang, Yun Liu, Da Wang, Huixin Zhang, Yechen An, Haijun Cheng, Jun Ma","doi":"10.1016/j.jhazmat.2025.139014","DOIUrl":"10.1016/j.jhazmat.2025.139014","url":null,"abstract":"<p><p>While non-radical Co species are recognized as critical intermediates in peroxymonosulfate (PMS)/Co(II) systems, their speciation and formation pathways remain under debate. In this study, Mn(II), characterized by well-defined redox behavior and mild reactivity toward radical species, was employed as a mechanistic probe to elucidate the activation mechanism of the PMS/Co(II) system under near-neutral conditions. Trace Co(II) (1 µM) accelerated Mn(II) oxidation kinetics by over 2000-fold at pH 8.0 compared to PMS alone. Scavenging experiments and near-100 % PMS utilization efficiency confirmed a non-radical mechanism. Co(IV) was proposed as the primary reactive species. Mn(III) capture experiments and density functional theory calculations indicated that Co(IV) oxidized Mn(II) via single-electron transfer. The derived Co(III) byproduct further contributed to Mn(II) oxidation, with reaction rates of 1.06 × 10<sup>5</sup> M<sup>-1</sup>·s<sup>-1</sup> at pH 5.5 and 1.20 × 10<sup>5</sup> M<sup>-1</sup>·s<sup>-1</sup> at pH 8.0. Kinetic modeling validated this pathway, quantifying the Co(IV)-Mn(II) reaction rates as 2.88 × 10<sup>6</sup> M<sup>-1</sup>·s<sup>-1</sup> (pH 5.5) and 2.57 × 10<sup>6</sup> M<sup>-1</sup>·s<sup>-1</sup> (pH 8.0). Under the experimental conditions, Co(III) and Co(IV) contributed comparably to Mn(II) oxidation. Mn(II)-probing experiments revealed that organic contaminant degradation was governed by substrate-dependent competition among three key reactive species: Co(II)-PMS complexes, high-valent cobalt species, and radicals. These findings provided mechanistic insights into PMS/Co(II) activation and further confirmed its potential for efficient manganese removal in water treatment.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"495 ","pages":"139014"},"PeriodicalIF":11.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144510072","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Christelle Nabintu Kajoka, Stephan Brosillon, Corine Reibel, Yacine Khadija Diop, Marcos Oliveira, Vincent Rocher, Ghassan Chebbo, Johnny Gasperi, Julien Le Roux
{"title":"Removal of pharmaceuticals through UV-C/Performic acid advanced oxidation process: Kinetics and identification of reactive species.","authors":"Christelle Nabintu Kajoka, Stephan Brosillon, Corine Reibel, Yacine Khadija Diop, Marcos Oliveira, Vincent Rocher, Ghassan Chebbo, Johnny Gasperi, Julien Le Roux","doi":"10.1016/j.jhazmat.2025.139016","DOIUrl":"10.1016/j.jhazmat.2025.139016","url":null,"abstract":"<p><p>Performic acid (PFA), widely recognized for its disinfectant properties in wastewater, shows selective and limited reactivity in oxidizing micropollutants. This study investigates the activation of PFA through UV-C photolysis to generate an advanced oxidation process (UV-C/PFA) and enhance the degradation of six pharmaceuticals: lidocaine, furosemide, sulfamethoxazole, diclofenac, acetaminophen, and carbamazepine. The synergy of UV-C photolysis with PFA enhances the removal of PFA-persistent pharmaceuticals. For instance, diclofenac, acetaminophen, and sulfamethoxazole, initially unreactive with PFA, were entirely degraded within ten minutes under UV-C/PFA in a phosphate buffer solution. This increased reactivity results from generated reactive species like hydroxyl (HO<sup>•</sup>), peroxyl (R-O<sup>•</sup>) radicals and singlet oxygen (<sup>1</sup>O<sub>2</sub>), confirmed by electron paramagnetic resonance, with HO<sup>•</sup> primarily originating from the background H<sub>2</sub>O<sub>2</sub> present in the PFA solution. While UV-C/PFA produced fewer HO<sup>•</sup> than UV-C/H<sub>2</sub>O<sub>2</sub>, it has distinct advantages through the selective action of <sup>1</sup>O<sub>2</sub> and R-O<sup>•</sup> in degrading some pharmaceuticals. <sup>1</sup>O<sub>2</sub> was also detected in the PFA solution and could explain its selective reactivity, especially with compounds containing reduced sulfur or tertiary amine groups. Overall, UV-C/PFA yields transformation products of lower molar mass compared to PFA, thus potentially increasing mineralization. In wastewater effluent, UV-C/PFA improved pharmaceutical degradation, though scavenging effects by wastewater constituents reduced removal rates.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"495 ","pages":"139016"},"PeriodicalIF":11.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144565581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jun Li, Hailing Zhao, Yi Ren, Chao Liu, Longguo Li, Bo Lai
{"title":"Peracetic acid concentration-driven active species switching in sulfur-modified iron-doped graphitic carbon nitride for adaptive degradation of organics.","authors":"Jun Li, Hailing Zhao, Yi Ren, Chao Liu, Longguo Li, Bo Lai","doi":"10.1016/j.jhazmat.2025.139063","DOIUrl":"10.1016/j.jhazmat.2025.139063","url":null,"abstract":"<p><p>Herein, a sulfur-modified iron-doped g-C<sub>3</sub>N<sub>4</sub> composite (FSCN) was synthesized to activate peracetic acid (PAA) for organic micropollutant degradation. The FSCN/PAA system demonstrated exceptional catalytic performance surpassing control catalysts, achieving effective removal of multiple contaminants containing diverse electron-donating and -withdrawing functional groups. The results of quenching experiments and spectroscopic characterization analyses revealed concentration-dependent active species generation: hydroxyl radicals (HO<sup>•</sup>) predominated at low PAA concentrations (25 μM), whereas high-valent iron species (Fe(IV/V)) became dominant at elevated PAA levels (400 μM). This distinctive switching behavior stems from the dual catalytic functionality of FSCN, which simultaneously activates PAA to generate Fe(IV/V) while catalyzing H<sub>2</sub>O<sub>2</sub> decomposition to produce HO<sup>•</sup>. The practicability of FSCN/PAA system was systematically validated through real wastewater treatment and continuous flow operation, and the results indicate that the system showed robust environmental compatibility. This work establishes a novel concentration-dependent active species regulation strategy through rational catalyst design and PAA dosage control, providing fundamental insights and technological advancement for advanced oxidation processes in water remediation.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"495 ","pages":"139063"},"PeriodicalIF":11.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144568278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yi Lian Yin, You Xing Xu, Meng Ting Wang, Dao Zhi Yang, Xiao Yan Wang, Xian Ke Zhou, Meng Meng Huang, Shun Yang, Hui Fei
{"title":"Integrative analysis of microbiome and metabolome reveals the effect of deoxynivalenol on growth performance, liver and intestinal health of largemouth bass (Micropterus salmoides).","authors":"Yi Lian Yin, You Xing Xu, Meng Ting Wang, Dao Zhi Yang, Xiao Yan Wang, Xian Ke Zhou, Meng Meng Huang, Shun Yang, Hui Fei","doi":"10.1016/j.jhazmat.2025.139148","DOIUrl":"10.1016/j.jhazmat.2025.139148","url":null,"abstract":"<p><p>This study explored the toxic effects of deoxynivalenol (DON) intake at low (100 µg·Kg<sup>-1</sup>, LD group) and high doses (300 µg·Kg<sup>-1</sup>, HD group) on largemouth bass (Micropterus salmoides). After a 56-day feeding trial, the HD group exhibited significantly reduced growth performance and weakened antioxidant capacity, along with elevated activities of enzymes related to metabolic dysregulation. Histopathological analysis showed an increase in hepatic cell vacuoles, as well as a shortened intestinal villi in both LD and HD groups. Notably, high-dose DON intake markedly down-regulated the expression of intestinal epithelial tight junction-related genes and proteins. Microbiome analysis indicated a significant increase in the Delftia and Acinetobacteria relative abundance, accompanied by diminished in Mycoplasma abundance in the HD group. Metabolomic profiling demonstrated that the dysregulated metabolites were mainly associated with the lysine biosynthesis pathway. Integrative multi-omics analysis revealed that pyridoxamine and diferuloylputrescine served as key biomarkers associated with Acinetobacteria. Collectively, we confirmed that high-dose DON intake induces hepatointestinal damage, thereby impairing the growth performance of largemouth bass. Our findings also further highlighted the link between DON-induced gut microbiota alterations and metabolic disorders, offering new intervention targets for alleviating DON toxicity.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"495 ","pages":"139148"},"PeriodicalIF":11.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144577448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yangqi E, Binyao Wang, Yibo Lin, Huachang Jin, Xueming Chen, Jianmeng Chen, Jin Hur, Yang Yu, Dongzhi Chen
{"title":"Electro-pulsation-generated variable-valent metal triggers alternate pesticide oxidation-chlorinated byproduct reduction on ruthenium-single-atom electrode.","authors":"Yangqi E, Binyao Wang, Yibo Lin, Huachang Jin, Xueming Chen, Jianmeng Chen, Jin Hur, Yang Yu, Dongzhi Chen","doi":"10.1016/j.jhazmat.2025.139052","DOIUrl":"10.1016/j.jhazmat.2025.139052","url":null,"abstract":"<p><p>Anodic oxidation presents a compelling strategy for pesticide-contained wastewater treatment. However, due to the reactive chlorine species-induced side reactions, toxic chlorinated byproducts are prevalent. Herein, a MOF derivative Ru-single-atom electrode, Ru-SbO<sub>X</sub>, was specialized for use in electro-pulsation to realize pesticide degradation and in-situ byproduct elimination. The introduction of single-atomic Ru promoted pseudocapacitive Ru<sup>n+</sup>-Sb<sup>n+</sup> redox conversion, electro-creating metastable high-valent Sb<sup>5+</sup> and low-valent Sb<sup>3+</sup>, then triggering the •OH and •H generation during anodic and cathodic cycles, respectively. This beneficially created an alternating oxidation-reduction environment in an identical electrode, leading to alternate pesticide degradation-byproduct elimination. These allowed Ru-SbO<sub>X</sub> to achieve a super-prominent normalized phoxim degradation kinetics constant (3.1 × 10<sup>-6</sup> m·s<sup>-1</sup>) in anodic cycles, surpassing other state-of-the-art electrodes; meanwhile, the reactive chlorine species-induced chlorinated byproducts and even N, S, P-related byproducts were in-situ eliminated by at least 10 times in cathodic cycles. This work provides a new perspective for tuning the valence-variable metal in the single-atom electrode to achieve efficient pesticide degradation and in-situ byproduct elimination using the electro-pulsation method.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"495 ","pages":"139052"},"PeriodicalIF":11.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144512978","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}