Journal of hazardous materials最新文献

Photodegradation process and mechanism of 2,3,6-trichloronaphthalene on kaolinite surfaces under ultraviolet-A irradiation: Role of fulvic acid and density functional theory calculations.

Journal of hazardous materials Pub Date : 2025-02-07 DOI: 10.1016/j.jhazmat.2025.137481

YingTan Yu, WenBo Si, Shumeng Zhao, ShiMeng Wang, MengDi Liu, Bing Fan, Shuang Xue, Jian Wang, Jing Xu

{"title":"Photodegradation process and mechanism of 2,3,6-trichloronaphthalene on kaolinite surfaces under ultraviolet-A irradiation: Role of fulvic acid and density functional theory calculations.","authors":"YingTan Yu, WenBo Si, Shumeng Zhao, ShiMeng Wang, MengDi Liu, Bing Fan, Shuang Xue, Jian Wang, Jing Xu","doi":"10.1016/j.jhazmat.2025.137481","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2025.137481","url":null,"abstract":"Polychlorinated naphthalenes (PCNs), a class of persistent organic pollutants (POPs), pose significant environmental and health risks, with trichloronaphthalene being a predominant congener in atmospheric particulate matter. This study investigates the photodegradation of 2,3,6-trichloronaphthalene (CN-26) on kaolinite surfaces under ultraviolet-A (UV-A) irradiation, focusing on the impact of fulvic acid (FA), temperature, humidity, and pH. The photodegradation mechanism of CN-26 was inferred via radical quenching experiments and density functional theory (DFT) calculations. The optimized degradation rate of CN-26 was 75.57 % at 25 °C, 70 % humidity, and pH 7 when FA was added at a concentration of 30 mg kg-1. Based on the radical quenching experiments, •OH are the primary active species involved in the degradation of CN-26, followed by electrons. In the absence of FA, •OH contributed 82.21 %, while electronic was 17.79 %. Conversely, in the presence of FA, the contribution rates of •OH, and electronic are 68.32 % and 21.21 % respectively. DFT calculations indicated that the 6 C site of CN-26 exhibited the highest susceptibility to radical attack, with the highest FED2HOMO+FED2LUMO value (0.25273), corroborated by averaged local ionization energy (ALIE) analysis. In the analysis of the reaction of •OH with CN-26, the lowest transition state ΔrG value of 1.09 kcal mol-1 was observed for compound 6 C, indicating that this site is the most susceptible to •OH attack. The degradation products of CN-26 were detected using gas chromatography-mass spectrometry (GC-MS), and the possible photodegradation pathways were proposed, which included dechlorination, hydroxylation, and aromatic ring opening. This study would provide insights into the photochemical behaviors of PCNs.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"488 ","pages":"137481"},"PeriodicalIF":0.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375066","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}

引用次数: 0

Regulating the electronic structure of iron sites in single-atom catalyst with interfacial chemical bond to enhance Fenton-like reaction.

Journal of hazardous materials Pub Date : 2025-02-07 DOI: 10.1016/j.jhazmat.2025.137483

Hongyu Shi, Hang Zhang, Tianyu Wang, Shuo Chen

{"title":"Regulating the electronic structure of iron sites in single-atom catalyst with interfacial chemical bond to enhance Fenton-like reaction.","authors":"Hongyu Shi, Hang Zhang, Tianyu Wang, Shuo Chen","doi":"10.1016/j.jhazmat.2025.137483","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2025.137483","url":null,"abstract":"Single-atom Fenton-like catalysts have been proven to be more efficient compared with aggregated catalysts due to abundant active sites. However, the low reduction rate of Fe(III) to Fe(II) remained the rate-limiting step for single-atom Fenton-like catalysts. Herein, carbon nanotubes with electron-withdrawing groups (CNTs-COOH) were combined with a single-atom catalyst (FeSAC) to fabricate a novel catalyst (FeSAC/CNTs-COOH, FCC-x). The optimal FCC-5/H2O2 system exhibited a 6.8 times higher pseudo-first-order kinetic constant of SMX degradation than that in FeSAC/H2O2 system. Additionally, the FCC-5/H2O2 system could maintain high catalytic activity within a wide pH range (4-9). The results of experiments and calculations co-verified the formation of Fe-O bonds between CNTs-COOH and FeSAC, which significantly reduced the electronic density of Fe(III) sites and further accelerated Fe(III) reduction to Fe(II), hence boosted the Fenton reaction. Quenching experiments and EPR measurements confirmed that hydroxyl radicals (⋅OH) were the primary active species responsible for pollutant degradation. The degradation pathway and toxicity analysis indicated that FCC-5/H2O2 was an eco-friendly reaction system. This study will provide a promising method for enhancing the performance of single-atom Fenton-like catalysts and offers insights into the underlying mechanisms.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"488 ","pages":"137483"},"PeriodicalIF":0.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375067","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}

引用次数: 0

Gene biomarkers in estuarine oysters indicate pollution profiles of metals, brominated flame retardants, and poly- and perfluoroalkyl substances in and near the Laizhou Bay. 河口牡蛎的基因生物标志物显示了莱州湾及其附近地区的金属、溴化阻燃剂、多氟和全氟烷基物质污染概况。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-11-12 DOI: 10.1016/j.jhazmat.2024.136484

Changlin Song, Liping You, Jianhui Tang, Shuang Wang, Chenglong Ji, Junfei Zhan, Bo Su, Fei Li, Huifeng Wu

{"title":"Gene biomarkers in estuarine oysters indicate pollution profiles of metals, brominated flame retardants, and poly- and perfluoroalkyl substances in and near the Laizhou Bay.","authors":"Changlin Song, Liping You, Jianhui Tang, Shuang Wang, Chenglong Ji, Junfei Zhan, Bo Su, Fei Li, Huifeng Wu","doi":"10.1016/j.jhazmat.2024.136484","DOIUrl":"10.1016/j.jhazmat.2024.136484","url":null,"abstract":"The Laizhou Bay (LZB) is of ecological and fishery importance. The discharge of effluents containing numerous pollutants into the LZB via rivers poses significant risks to ecosystem and human health. Estuarine biomonitoring is therefore crucial for assessing the contribution of rivers to coastal pollution and their impacts on species. Estuarine oyster Crassostrea gigas is a preferable bioindicator to pollution conditions. This study measured accumulation of contaminants and expression levels of gene biomarkers in the LZB and Northern Shandong Peninsula (NSP) oysters. The LZB oysters accumulated higher levels of brominated flame retardants (BFRs) and poly- and perfluoroalkyl substances (PFAS), while NSP oysters exhibited greater accumulation of heavy metals. Decabromodiphenyl ethane was the dominant BFR, while perfluorooctanoic acid and perfluoro-2-methoxyacetic acid were the dominant PFASs in oysters. The expression of gene biomarkers effectively distinguished the LZB and NSP oysters, with CYP2 subfamilies expression correlating with BFRs and PFASs and metallothionein expression indicating heavy metals. The reproductive endocrine and neuroendocrine-immune systems in oysters might be the targets of BFRs and heavy metal pollution, respectively. The negative correlation between contaminant accumulation and gene expression might be explained by adaptive evolution, emphasizing the need to consider genetic diversity in ecological risk assessments.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136484"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142635221","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}

引用次数: 0

Square-wave pulsed potential driven electrocatalytic degradation of 4-chlorophenol using Fe-Ni/rGO/PPy@NF three dimensional electrode. 使用 Fe-Ni/rGO/PPy@NF 三维电极对 4-氯苯酚进行方波脉冲电位驱动电催化降解。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-10-04 DOI: 10.1016/j.jhazmat.2024.136054

Bei Ma, Bobing Lu, Hanyu Tang, Hui Wang, Zhaoyong Bian

{"title":"Square-wave pulsed potential driven electrocatalytic degradation of 4-chlorophenol using Fe-Ni/rGO/PPy@NF three dimensional electrode.","authors":"Bei Ma, Bobing Lu, Hanyu Tang, Hui Wang, Zhaoyong Bian","doi":"10.1016/j.jhazmat.2024.136054","DOIUrl":"10.1016/j.jhazmat.2024.136054","url":null,"abstract":"To develop an energy-efficient system for the removal of chlorinated organic pollutants, Fe-Ni/reduced graphite oxide/polymerized polypyrrole@nickel foam was constructed as a catalytic cathode for pulsed electrocatalytic degradation, where cathode-catalyzed production of hydrogen radicals (H*) and hydroxyl radical (·OH) generated at the anode led to dechlorination of 4-chlorophenol (4-CP), and dechlorination products were mineralized and degraded under the action of·OH. When energy was continuously supplied to the reaction system in the constant potential mode, the 4-CP concentration near the electrode was insufficient, limiting the reaction rate. Conversely, in the square-wave pulsed potential mode, mass transfer limitations were mitigated, significantly enhancing reaction efficiency and reducing energy consumption. At -1.2 V (vs. Ag/AgCl), the 4-CP removal efficiency reached 93.79 % in the pulsed potential mode, surpassing the constant potential mode's performance of 81.40 %. The synergistic periodic oscillation of the potential, direct electron transfer, and catalytic generation of active free radicals in the pulsed potential mode reduced intermediate concentrations and increased 4-CP mineralization, while the degradation pathway remained unchanged. This research presents a method for the efficient treatment of chlorinated organic pollutants in water using pulsed electrocatalytic degradation.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136054"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142378741","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}

引用次数: 0

Gut microbiota modulation by L-Fucose as a strategy to alleviate Ochratoxin A toxicity on primordial follicle formation. 用L-岩藻糖调节肠道微生物群，减轻赭曲霉毒素A对原始卵泡形成的毒性。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-11-12 DOI: 10.1016/j.jhazmat.2024.136469

Ruiting Wang, Jie Song, Muyu Cai, Yuan Xue, Jing Liu, Ning Zuo, Massimo De Felici, Junjie Wang, Wei Shen, Xiaofeng Sun

{"title":"Gut microbiota modulation by L-Fucose as a strategy to alleviate Ochratoxin A toxicity on primordial follicle formation.","authors":"Ruiting Wang, Jie Song, Muyu Cai, Yuan Xue, Jing Liu, Ning Zuo, Massimo De Felici, Junjie Wang, Wei Shen, Xiaofeng Sun","doi":"10.1016/j.jhazmat.2024.136469","DOIUrl":"10.1016/j.jhazmat.2024.136469","url":null,"abstract":"In this study, we investigated the potential benefits of L-Fucose administration to pregnant mice exposed to Ochratoxin A (OTA), a widespread mycotoxin, producing ovarian damage in offspring. The results showed that administration of 3.5 μg/d OTA induced alterations in intestinal tissues and gut microbiota of pregnant mice, leading to heightened local and systemic inflammation. This inflammatory affected the ovaries of their 3 dpp offspring, in which elevated levels of LPS and ROS were found associated to significant decreased oocyte count and impaired primordial follicle assembly. Moreover, mRNA-Seq analysis showed significant changes in ovarian transcriptomes linked to various GO terms and KEGG pathways, notably ferroptosis, a recognized form of cell death observed. Interestingly, administration of 0.3 g/kg b. w. L-Fucose following OTA exposure mitigated these effects on intestinal tissues and gut microbiota in mothers and on the offspring's ovaries. Similar benefits were obtained by gut microbiota transplantation from L-Fucose-treated pregnant females into OTA-exposed mothers. These findings suggest that inflammatory impact of OTA on maternal intestine/gut can pass to the fetus causing offspring ovary defects and support the use of L-Fucose as adjuvant to counteract the adverse effects of mycotoxins on the gut microbiota, particularly reference to those affecting reproductive organs.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136469"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142635223","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}

引用次数: 0

The successive reduction of iodate to iodide driven by iron redox cycling. 在铁氧化还原循环的驱动下，碘酸根连续还原成碘化物。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-11-08 DOI: 10.1016/j.jhazmat.2024.136436

Siqi Zhu, Zhou Jiang, Yongguang Jiang, Yiran Dong, Junxia Li, Liang Shi

{"title":"The successive reduction of iodate to iodide driven by iron redox cycling.","authors":"Siqi Zhu, Zhou Jiang, Yongguang Jiang, Yiran Dong, Junxia Li, Liang Shi","doi":"10.1016/j.jhazmat.2024.136436","DOIUrl":"10.1016/j.jhazmat.2024.136436","url":null,"abstract":"Ferrous iron (Fe(II)) produced by microbial Fe(III) reduction and reactive oxygen species (ROS) generated from aerobic Fe(II) oxidation can mediate iodate (IO3-) reduction and iodide (I-) oxidation, respectively. Nevertheless, how Fe redox cycling under redox fluctuating conditions drives transformation of iodine species remain unclear. In this study, Shewanella oneidensis MR-1 wildtype (WT) and its mutant △dmsEFAB, which lost the ability to enzymatically reduce IO3-, were chosen to conduct ferrihydrite/goethite/nontronite culture experiments under consecutive cycles of anoxic reduction of Fe(III) and re-oxidation of Fe(II) by O2 to reveal the role of Fe redox cycling in the transformation of iodine species. The results showed that both surface-adsorbed and mineral structural Fe(II) chemically reduced IO3-. Chemical IO3- reduction by biogenic Fe(II) was slower than enzymatic IO3- reduction by WT. Compared to △dmsEFAB cultures, WT cultures all showed higher Fe(II) concentrations under anoxic conditions but lower cumulative •OH under oxic conditions, which imply the chemical reaction between I- and ROS. I- oxidation by ROS, however, did not lead to a significant production of IO3- compared with I- formed under anoxic conditions. Consequently, Fe redox cycling successively reduced IO3- to I-, which highlights vital roles of Fe(III)-reducing bacteria in I- formation and mobilization in environments.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136436"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142635231","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}

引用次数: 0

Revealing the essence of anion ligands in regulating amorphous MnOx to activate peracetic acid for micropollutant removal. 揭示阴离子配体在调节无定形氧化锰活化过乙酸以去除微污染物方面的本质。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-10-31 DOI: 10.1016/j.jhazmat.2024.136361

Yudan Dong, Si Sun, Yunzhe Zheng, Jiamei Liu, Peng Zhou, Zhaokun Xiong, Jing Zhang, Zhi-Cheng Pan, Chuan-Shu He, Bo Lai

{"title":"Revealing the essence of anion ligands in regulating amorphous MnOx to activate peracetic acid for micropollutant removal.","authors":"Yudan Dong, Si Sun, Yunzhe Zheng, Jiamei Liu, Peng Zhou, Zhaokun Xiong, Jing Zhang, Zhi-Cheng Pan, Chuan-Shu He, Bo Lai","doi":"10.1016/j.jhazmat.2024.136361","DOIUrl":"10.1016/j.jhazmat.2024.136361","url":null,"abstract":"How the anion ligands of manganese precursors affect the catalytic activity of amorphous manganese oxides (MnOx) in Fenton-like process is poorly understood. Here, five amorphous MnOx synthesized by Mn(II) precursors with different ligands were characterized and adopted to activate peracetic acid (PAA) for bisphenol A (BPA) degradation. Although > 90 % BPA removal was achieved in the five MnOx/PAA processes via both adsorption and oxidation, the oxidation kobs greatly differentiates by the ligands types with the order of MnOx-N > MnOx-S > MnOx-Cl > MnOx-AA > MnOx-OA. Ligands types would affect the specific surface area of MnOx and their ability to adsorb BPA, however which is not the decisive factor in determining the contaminant oxidation efficiency. Multiple experimental results indicate that the generation of oxygen vacancies induced by the ligands alters the Mn(III)/Mn(IV) ratio, ultimately contributing to the different efficiency of BPA oxidation driven by the direct electron transfer mechanism. Moreover, amorphous MnOx holds the promise of practical applications in catalytic PAA of various micropollutants with good stability. This study advances the fundamental understanding of ligand-regulated amorphous MnOx-catalyzed PAA process.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136361"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565383","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}

引用次数: 0

Biochar-bacteria coupling system enhanced the bioremediation of phenol wastewater-based on life cycle assessment and environmental safety analysis. 基于生命周期评估和环境安全分析的生物炭-细菌耦合系统增强了苯酚废水的生物修复能力。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-11-05 DOI: 10.1016/j.jhazmat.2024.136414

Xuejiao An, Yanlin Wang, Chenglong Yu, Xiaojing Hu

{"title":"Biochar-bacteria coupling system enhanced the bioremediation of phenol wastewater-based on life cycle assessment and environmental safety analysis.","authors":"Xuejiao An, Yanlin Wang, Chenglong Yu, Xiaojing Hu","doi":"10.1016/j.jhazmat.2024.136414","DOIUrl":"10.1016/j.jhazmat.2024.136414","url":null,"abstract":"The efficient treatment of phenol wastewater is of great necessity since it induces serious pollution of water and soil ecosystems. Using biochar-immobilized functional microorganisms can innovatively and sustainably deal with the existing problem. In this study, we utilized response surface methodology (RSM) combined with life cycle assessment (LCA) to improve phenol biodegradation rate through a novel separated alkali-resistant and thermophilic strain Bacillus halotolerans ACY. Bioinformatic analysis revealed the genetic foundation of ACY to adapt to harsh environments. The characteristics of pig manure biochar (PMB) produced at varying pyrolysis temperatures (300-700 ℃) and adsorption experiment were investigated, immobilization of the phenol-degrading ACY on PMB600 under alkaline and high pollution load promoted phenol removal and extreme environment resistance, and the phenol removal rate reached 99.5 % in 7d in actual phenol wastewater, which increased compared with those achieved by PMB (50.6 %) and free bacteria (80.5 %) alone. Scanning Electron Microscope (SEM) and Fourier transform infrared spectrometry (FTIR) observations indicated the successful bacterial immobilization on PMB600. Reusability and economic cost study further demonstrated PMB600 as an excellent carrier for wastewater treatment. LC-MS, toxicology and carbon footprint analyses demonstrated that bacterial metabolism exerted synergy with adsorption for phenol removal, while biodegradation exerted the predominant impact on the immobilized bacterial system. This study provides an eco-friendly and effective approach to treat phenol wastewater.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136414"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142607836","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}

引用次数: 0

Antimony-bearing schwertmannite transformation to goethite: A driver of antimony mobilization in acid mine drainage. 含锑的闪长岩转变为网纹石：酸性矿井排水中锑迁移的驱动因素。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-11-12 DOI: 10.1016/j.jhazmat.2024.136487

Mohammad Rastegari, Niloofar Karimian, Scott G Johnston, Girish Choppala, Mona Hosseinpour Moghaddam, Edward D Burton

{"title":"Antimony-bearing schwertmannite transformation to goethite: A driver of antimony mobilization in acid mine drainage.","authors":"Mohammad Rastegari, Niloofar Karimian, Scott G Johnston, Girish Choppala, Mona Hosseinpour Moghaddam, Edward D Burton","doi":"10.1016/j.jhazmat.2024.136487","DOIUrl":"10.1016/j.jhazmat.2024.136487","url":null,"abstract":"Antimony(V) mobility in acid mine drainage (AMD) is often controlled by sorption and coprecipitation with schwertmannite - a poorly-ordered Fe(III) oxyhydroxysulfate mineral. However, due to its metastable nature, schwertmannite transforms over time to more thermodynamically stable Fe(III) phases, such as goethite. This study examines how transformation of Sb(V)-bearing schwertmannite to goethite impacts Sb(V) mobility, while also assessing the role that Sb(V) may play in stabilizing schwertmannite against such transformation. To address these aims, Sb(V)-free, Sb(V)-sorbed and Sb(V)-coprecipitated schwertmannite were allowed to undergo partial transformation to goethite under acid sulfate conditions. Iron K-edge EXAFS spectroscopy revealed that sorbed and coprecipitated Sb(V) partly stabilized schwertmannite against transformation. The onset of schwertmannite transformation to goethite was found to drive clear mobilization of Sb(V) into solution, regardless of the Sb(V) loading or whether Sb(V) was initially sorbed or coprecipitated with the precursor schwertmannite. This initial phase of Sb(V) mobilization was followed by subsequent solid-phase recapture of the released Sb(V), with Sb K-edge EXAFS spectroscopy revealing that this process involved Sb(V) incorporation into the newly-formed goethite. Our findings show that, although schwertmannite transformation to goethite is partially inhibited by co-existing Sb(V), the initial stage of this transformation process drives significant Sb(V) mobilization in AMD systems.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136487"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142635204","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}

引用次数: 0

pH dependence of reactive oxygen species generation and pollutant degradation in Fe(II)/O₂/tripolyphosphate system. Fe(II)/O2/tripolyphosphate 系统中活性氧生成和污染物降解的 pH 值依赖性。

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-10-16 DOI: 10.1016/j.jhazmat.2024.136174

Chengwu Zhang, Anqi Yang, Bing Qin, Wei Zhao, Chuipeng Kong, Chuanyu Qin

{"title":"pH dependence of reactive oxygen species generation and pollutant degradation in Fe(II)/O2/tripolyphosphate system.","authors":"Chengwu Zhang, Anqi Yang, Bing Qin, Wei Zhao, Chuipeng Kong, Chuanyu Qin","doi":"10.1016/j.jhazmat.2024.136174","DOIUrl":"10.1016/j.jhazmat.2024.136174","url":null,"abstract":"It has been reported that tripolyphosphate (TPP) can effectively enhance the activation of O2 by Fe(II) to remove organic pollutants in the environment. However, the influence of solution pH on the generation and conversion of reactive oxygen species (ROS) and their degradation of pollutants in the Fe(II)/O2/TPP system needs further investigation. In this study, we demonstrated that O2•- and •OH were the main ROS responsible for degradation in the system at different pH conditions, and their formation rates were calculated using a steady-state model. Experiments combined with density functional theory (DFT) calculations showed that the p-nitrophenol (PNP) degradation pathway in the Fe(II)/O2/TPP system is regulated by solution pH. Specifically, at pH = 3, the existence of Fe(II) in the solution is dominated by [Fe(II)(HTPP)2]2-, which leads to a rapid conversion from O2 and HO2• to generate •OH, and PNP is primarily oxidatively degraded. However, at pH = 5/7, [Fe(II)(TPP)2]4- is taking the lead with which O2•- is accumulated in the solution due to the slow conversion to •OH in this condition, and the PNP is mainly reductively degraded. This study proposes a new strategy to achieve the targeted oxidative/reductive removal of different types of pollutants by simply varying the solution pH in the Fe(II)/O2/TPP system.","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":"480 ","pages":"136174"},"PeriodicalIF":0.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142484210","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}

引用次数: 0