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AQDS Enhances Degradation of BDE-47 by Promoting Shewanella oneidensis MR-1-mediated Fenton Reaction with Fe(III)-containing Minerals

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Journal of Earth Science 2025年

作者： Yongguang Jiang Siqi Zhu Zhou Jiang Yiran Dong Liang Shi School of Environmental Studies， China University of Geosciences State Key Laboratory of Biogeology and Environmental Geology， China University of Geosciences Hubei Key Laboratory of Yangtze Catchment Environmental Aquatic Science， China University of Geosciences State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic Pollution， Ministry of Ecology and Environment， China University of Geosciences(Wuhan)

Electron shuttles are widespread in the environments and play important role in microbe-mineral interaction. This study investigated the effects of a model electron shuttle (i.e.， anthraquinone-2， 6-disulfonate， AQDS) on Shewanella oneidensis MR-1-mediated Fenton reaction and subsequent degradation of 2， 2′， 4， 4′-tetrabrominated diphenyl ether (BDE-47). Three Fe(III)-containing minerals， namely， ferrihydrite， goethite and nontronite， were used as electron acceptors and Fe(II) sources. With each mineral， additions of 0.01 – 1 mM AQDS in the reactions significantly enhanced Fe(III) reduction by S. oneidensis MR-1 and increased the amounts of Fe(II) produced in anoxic phase. As a result， the amounts of cumulative ·OH formed in oxic phase were increased by 10% – 287%. Regression analysis revealed that ·OH cumulation has significant linear correlation with sorbed Fe(II) but not aqueous and structural Fe(II). This finding may be ascribed to the higher reactivity of sorbed Fe(II) in oxygenation than the latter two types of Fe(II). With more ·OH， the degradation efficiency of BDE-47 was elevated by 31% – 173%. Collectively， AQDS enhances ·OH formation and BDE-47 degradation by promoting production of Fe(II)， particularly sorbed Fe(II) in S. oneidensis MR-1-mediated Fenton reaction with Fe(III)-containing minerals.

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FeCoP sub-nanometric-sheets for electrocatalzing overall water splitting

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Nano Research Energy 2024年第4期3卷 68-76页

作者： Long Zhao Kexin Meng Yibo Guo Qingsheng Wu Quanjing Zhu Tao Zhou Yongqing Fu Ming Wen School of Chemical Science and Engineering School of Environmental Science and EngineeringShanghai Key Laboratory of Chemical Assessment and SustainabilityState Key Laboratory of Pollution Control and Resource ReuseTongji UniversityShanghai 200092China College of Bioengineering East China University of Science and TechnologyShanghai 200237China Faculty of Engineering and Environment Northumbria UniversityNewcastle upon Tyne NE99UK

Renewable electrical energy for electrolysis water can achieve green industrial chains for hydrogen ***,finding efficient electrocatalysts remains a challenge for green ***,sub-nanometric FeCoP nanosheets with average thickness of 0.9 nm is constructed through 2D self-assembly driven by cavitation effect of ultrasonics and following *** from abundant active sites,enhanced H_(2)O molecular adsorption kinetics,and highly enhanced structural stability,the subcrystalline FeCoP shows excellent electrocatalytic activities of hydrogen evolution reaction(HER)and oxygen evolution reactions(OER).Ultralow overpotential of 37 mV is achieved at 10 mA·cm^(-2) for *** the FeCoP catalyst was used as both cathode and anode for overall water splitting using renewable electrical energy,green hydrogen produced is directly applied for hydrogen fuel cell to drive fan for more than 10 *** calculation indicates that subcrystalline FeCoP more easily adsorbs H_(2)O than crystalline one and thus speeds up the kinetics of Volmer step in HER process.

关键词： green hydrogen energy subcrystalline overall water splitting sub-nanometric-sheets

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Interactions between methyl octabromo ether flame retardant and expanded polystyrene microplastics in the photoaging process

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Chemosphere 2024年 358卷 142165页

作者： Shi, Yanqi Zheng, Lezhou Huang, Hexinyue Shi, Linping Gong, Zhimin Ye, Kefu Chen, Xingqi Gao, Shixiang State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu Nanjing210093 China

Expanded polystyrene (EPS) plastic is widely used because of its low density and lightweight properties, enabling it to float on water and increase its exposure to sunlight. In this study, we simulated the photoaging process of flame retardant-added EPS (FR-EPS) and common original EPS (OR-EPS) microplastic (MP) particles with and without methyl octabromoether flame retardant (MOBE) in the laboratory to explore the effect of MOBE on the photodegradation of EPS. Results showed that MOBE accelerated size reduction and surface hole formation on the particles, hastening the shedding and replacement of particle surfaces. FR-EPS particles exhibited a weight loss exceeding that of OR-EPS, reaching 40.85 ± 3.72% after 36 days of irradiation. Moreover, rapid physical peeling of the FR-EPS surface was accompanied by continuous chemical oxidation and fluctuations of the carbonyl index and O/C ratio. A diffusion model based on Fick's second law fitted well for the concentration of MOBE remaining in FR-EPS particles. MOBE's sensitivity to direct photochemical reactions inhibited the early-stage photoaging of EPS MP particles by competing for photons. However, MOBE as chromophores could absorb photons and produce •OH to promote the aging of EPS. Moreover, the capacity of EPS to absorb light energy also accelerated MOBE degradation. These findings suggested that the photoaging behavior of commercial EPS products containing flame retardants in the environment is quite different from that of pure EPS, indicating that additive-plastic interactions significantly alter MP fate and environmental risks. © 2024 Elsevier Ltd

关键词： Microplastic

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Modification strategies on 2D Ni-Fe MOF-based catalysts in peroxydisulfate activation for efficient organic pollutant removal

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Chinese Chemical Letters 2023年第4期34卷 406-409页

作者： Minjun Liu Ying Liu Xinru Liu Chengcheng Chu Ducheng Yao Shun Mao College of Environmental and Chemical Engineering Shanghai University of Electric PowerShanghai 200090China College of Environmental Science and Engineering Biomedical Multidisciplinary Innovation Research InstituteShanghai East HospitalState Key Laboratory of Pollution Control and Resource ReuseTongji UniversityShanghai 200092China

This study reports several modification strategies to optimize and enhance the performance of twodimensional(2D) metal organic frameworks(MOFs)-derived catalysts in peroxydisulfate(PDS) *** raw 2D Ni-MOF and 2D Ni-Fe-MOF without modification show poor catalytic activities for PDS activation and high metal ion leaching. The carbonization of 2D MOF can increase the activity of the catalyst but cannot solve the metal leaching problem. The further acid treatment of carbonization products can further improve the catalytic activity and decrease the metal ion leaching. The in-situ growth of2D MOF on graphene oxide(GO) support with subsequent carbonization and acid treatment offers the best performance in PDS activation for organic pollutant removal with low metal ion leaching. Compared with other PDS systems, the Ni-Fe-C-acid/GO system displays much lower catalyst and PDS dosages for p-chloroaniline degradation. This study presents new insights in the modification strategies of 2D MOFbased catalysts in PDS activation.

关键词： Peroxydisulfate oxidation 2D MOF Modification strategy Synergistic effect Organic pollutant removal

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Mechanisms of allicin exposure for the sludge fermentation enhancement:Focusing on the fermentation processes and microbial metabolic traits

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Journal of Environmental Sciences 2022年第5期34卷 253-264页

作者： Feng Wang Jingyang Luo Shiyu Fang Wenxuan Huang Yunqi Zhang Le Zhang Xiaoshi Cheng Wei Du Fang Fang Jiashun Cao Yang Wu Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes Ministry of EducationHohai UniversityNanjing 210098China College of Environment Hohai UniversityNanjing 210098China State Key Laboratory of Pollution Control and Resource Reuse School of Environmental Science and EngineeringTongji UniversityShanghai 200092China

As a frequently used product with antimicrobial activity,consumed allicin might be dis-charged and concentrated in waste-activated sludge(WAS).However,the influence of al-licin(as an exogenous pollutant)on WAS fermentation has not been clearly *** study aimed to disclose the impacts of allicin on volatile fatty acid(VFA)generation dur-ing WAS *** results showed that the appropriate presence of allicin(10 mg/g TSS)significantly enhanced the VFA yield(1894 versus 575 mg COD/L in the control)with increased acetate proportion(24.3%).Further exploration found that allicin promoted WAS solubilization,hydrolysis and acidification *** analysis revealed that the key genes involved in extracellular hydrolysis metabolism(i.e.,CAZymes),mem-brane transport(i.e.,gtsA and ytfT),substrate metabolism(i.e.,yhdR and pfkC)and fatty acid synthesis(i.e.,accA and accD)were all highly *** also induced the bacteria to produce more signalling molecules and regulate cellular functions,thereby enhancing the microbial adaptive and regulatory capacity to the unfavourable ***,the variations in fermentative microbes and their contributions to the upregulation of func-tional genes(i.e.,ytfR,gltL,INV,iolD and pflD)for VFA generation were ***,the simultaneous stimulation of functional microbial abundances and metabolic activities contributed to VFA production in allicin-conditioned reactors.

关键词： Allicin Waste activated sludge(WAS) Anaerobic fermentation Metagenomic analysis Functional genes

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Evaluation of N-acetylcysteine and glutathione as quenching agents for the analysis of halogenated disinfection by-products

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Journal of Environmental Sciences 2022年第7期34卷 71-79页

作者： Shunke Ding Menglin Wu Rong Xiao Chao Fang Qi Wang Bin Xu Wenhai Chu State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Key Laboratory of Yangtze River Water Environment Ministry of EducationTongji UniversityShanghai 200092China School of Life and Environmental Science Wenzhou UniversityZhejiang 325035China

Disinfection by-products(DBPs), formed from the reactions of disinfectants with natural organic matter and halides in drinking water, were considered to be cytotoxic and genotoxic, and might trigger various cancers. The relatively low concentration of DBPs in finished water(low μg/L or even ng/L levels) and the interference from water matrix inhibited in situ determination of DBPs. Moreover, the further formation and degradation of DBPs by disinfectants during the holding time(several hours to several days) from sample collection to analysis could adversely affect the determination of DBPs. To obtain accurate, precise and reliable data of DBP occurrence and formation, robust and reliable sample preservation is indispensable. However, the commonly used quenching agents(e.g., sodium sulfite, sodium thiosulfate, and ascorbic acid) for sample preservation can decompose reactive DBPs by reductive dehalogenation. This study evaluated the performance of N-acetylcysteine(NAC) and glutathione(GSH) as quenching agents for the analysis of halogenated DBPs by investigating the stoichiometry of the disinfectant-quenching agent reaction, the formation of DBPs during chlor(am)ination of NAC or GSH, and the effects of NAC or GSH on the stability of 18 individual DBPs and total organic halogen(TOX). Based on the results of this study, NAC and GSH were considered to be ideal quenching agents for the analysis of most DBPs and TOX, except halonitromethanes.

关键词： Disinfection by-products Total organic halogen Quenching agents N-acetylcysteine Glutathione

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Water:The lifeblood of the Earth-human system revealed in elemental correlations

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Science China Earth Sciences 2023年第10期66卷 2386-2390页

作者： Zimeng WANG Yongsheng LIU Anhuai LU Yanxin WANG Department of Environmental Science and Engineering Fudan UniversityShanghai200433China State Key Laboratory of Geological Processes and Mineral Resources School of Earth SciencesChina University of GeosciencesWuhan430074China Beijing Key Laboratory of Mineral Environmental Function School of Earth and Space SciencesPeking UniversityBeijing100871China MOE Key Laboratory of Groundwater Quality and Health State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic PollutionSchool of Environmental StudiesChina University of GeosciencesWuhan430074China

*** and human history The rich chemistry of Earth's elements played an inherent and multifaceted role in shaping the course of human ***,the more inert an element is,the simpler it becomes to extract it from miner... 详细信息

关键词： Earth minerals simpler

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Enhanced oil/water separation using superhydrophobic nano SiO2-modified porous melamine sponges

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Chemosphere 2024年 369卷 143879页

作者： Chen, Yongsheng Xue, Yi Ma, Sijia Shi, Haochuan Wang, Yanru Ren, Hongqiang Xu, Ke State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu Nanjing210023 China

Recent advancements in functional sponge materials have garnered significant interest due to their efficacy and cost-effectiveness in oil spill remediation. This study introduces both silane coupling agent (methyltrichlorosilane and 3-aminopropyltriethoxysilane) and nano-SiO₂ particles into the melamine sponge framework via impregnation. Additionally, polydimethylsiloxane (PDMS) serves a crucial role in curing to fuse the substrate with the coating through robust covalent bonds. The modified sponges (SiMAPs) facilitate the formation of rough surfaces comprising hierarchical structures by the deposition of nano-SiO₂ particles, while the silane coupling agents and PDMS contribute to a reduced surface energy. These SiMAP sponges maintain high stability with a water contact angle of 162.6° and demonstrate an adsorption capacity ranging from 40 to 90 times their weight in oil or organic solvents. Furthermore, they achieve a separation efficiency exceeding 98% and an oil flux of 14.38 L/m2∙s in immiscible oil-water mixtures. Additionally, the sorption of trichloromethane reaches 88.1 g/g, and the separation efficiency for surfactant-stabilized emulsions containing diesel is 62.8%. Remarkably, the oil-water separation efficiency surpasses 99.8% in dynamic continuous oil-water separation cycles, as evidenced by 20 experimental trials. These results underscore the substantial potential of SiMAP-modified sponges for addressing oil pollution by enhancing oil-water separation. © 2024

关键词： Demulsification

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Highly efficient P uptake by Fe3O4 loaded amorphous Zr-La (carbonate) oxides: Electrostatic attraction, inner-sphere complexation and oxygen vacancies acceleration effect

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Journal of Environmental Sciences 2022年第10期34卷 18-29页

作者： Chenyang Liu Yili Wang Xiaolin Li Junyi Li Shuoxun Dong Haotian Hao Yao Tong Yanqing Zhou College of Environmental Science and Engineering Beijing Key Lab for Source Control Technology of Water PollutionBeijing Forestry UniversityBeijing 100083China Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China

Bimetallic oxides composites have received an increasing attention as promising adsorbents for aqueous phosphate (P) removal in recent years. In this study, a novel magnetic composite MZLCO was prepared by hybridizing amorphous Zr-La (carbonate) oxides (ZLCO) with nano-FeOthrough a one-pot solvothermal method for efficient phosphate adsorption. Our optimum sample of MZLCO-45 exhibited a high Langmuir maximum adsorption capacity of 96.16 mg P/g and performed well even at low phosphate concentration. The phosphate adsorption kinetics by MZLCO-45 fitted well with the pseudo-second-order model, and the adsorption capacity could reach 79% of the ultimate value within the first 60 min. The phosphate adsorption process was highly p H-dependent, and MZLCO-45 performed well over a wide p H range of 2.0-8.0. Moreover, MZLCO-45 showed a strong selectivity to phosphate in the presence of competing ions (Cl^(-), NO_(3)^(-), SO_(4)^(2-), HCO_(3)^(-), Ca^(2+), and Mg^(2+)) and a good reusability using the eluent of Na OH/Na Cl mixture, then 64% adsorption capacity remained after ten recycles. The initial 2.0 mg P/L in municipal wastewater and surface water could be efficiently reduced to below 0.1mg P/L by 0.07 g/L MZLCO-45, and the phosphate removal efficiencies were 95.7% and 96.21%, respectively. Phosphate adsorption mechanisms by MZLCO-45 could be attributed to electrostatic attraction and the inner-sphere complexation via ligand exchange forming Zr/La-O-P, -OH and CO_(3)^(2-)groups on MZLCO-45 surface played important roles in the ligand exchange process. The existence of oxygen vacancies could accelerate the phosphate absorption rate of the MZLCO-45 composites.

关键词： Fe3O4 loaded amorphous Zr-La(carbonate)oxides Phosphate adsorption performance Regeneration Mechanism Real water treatment

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冻融及耦合酸化作用下土壤中重金属的浸出性及其机制解析

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Journal of Central South University 2024年第4期31卷 1197-1206页

作者：付田雨李捷付融冰 State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Institute of Environmental and Municipal Engineering Qingdao University of TechnologyQingdao 266033China

冻融与不同pH溶液的耦合作用下土壤中重金属浸出行为尚缺乏研究。本研究采用TCLP测试评估了冻融及耦合酸化处理前后土壤中重金属的浸出毒性,并采用孔隙(颗粒)与裂隙图像识别与分析系统(PCAS)和地球化学模拟软件(PHREEQC)分别探究土壤矿... 详细信息

冻融与不同pH溶液的耦合作用下土壤中重金属浸出行为尚缺乏研究。本研究采用TCLP测试评估了冻融及耦合酸化处理前后土壤中重金属的浸出毒性,并采用孔隙(颗粒)与裂隙图像识别与分析系统(PCAS)和地球化学模拟软件(PHREEQC)分别探究土壤矿物颗粒的微观结构和矿物学演化特征。结果表明,经过30次冻融循环后,As、Cd、Cu、Mn、Pb和Zn的最大浸出浓度分别为0.22 mg/L、0.61 mg/L、2.46 mg/L、3.08 mg/L、29.36 mg/L和8.07 mg/L。在冻融和酸化的耦合作用下,土壤颗粒的孔隙度增加了4.79%。孔隙和裂缝的演化所引起的颗粒结构破坏证实了这一结果。在冻融作用下,土壤颗粒的各向异性增加,而在冻融与酸化的耦合作用下,土壤颗粒的各向异性降低。SEM-EDS、PCAS量化和PHREEQC模拟的结果表明,重金属的释放机制不仅与矿物颗粒的微观结构演化特征有关,还受质子腐蚀以及矿物的溶解和沉淀的影响。这些结果将为季节性冻土地区污染场地土壤修复评价提供重要参考。

关键词：污染土壤重金属浸出性冻融循环酸化孔隙(颗粒)与裂隙图像识别与分析系统(PCAS) PHREEQC软件

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