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Oxygen vacancy-modified fast charge transport channels at the interface of bismuth S-scheme heterojunctions promoting photocatalytic performance

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CHEMICAL ENGINEERING JOURNAL 2025年 506卷

作者： Liu, Jiawei Zhang, Zhilin Lin, Junhao Zhen, Li Jiang, Qingyang Shi, Jun Deng, Huiping Tongji Univ Shanghai Inst Pollut Control & Ecol Secur Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China

While oxygen vacancies (Ov) in single semiconductor photocatalysts have been extensively studied, investigations into and comprehensive understanding of electron transfer and intrinsic mechanisms of Ov in heterojunction photocatalysts-particularly S-scheme heterojunctions-remain inadequate. In this study, novel oxygen vacancy-rich Ov-Bi4O7/Bi3.64Mo0.36O6.55 (MOB) S-scheme heterojunction catalysts were designed and constructed. These catalysts combine oxygen vacancy-rich Bi4O7 with Bi3.64Mo0.36O6.55 (BMO) to enhance interfacial charge transfer across the heterojunction and generate active centers enriched with oxygen vacancies. The optimized MOB-32 heterojunction achieved 97.6% degradation of tetracycline (TC) under light irradiation. The introduction of Ov improved the local electronic structure and microenvironment of the S-scheme heterojunction. Femtosecond transient absorption spectroscopy (Fs-TAS) reveals that Ov introduces additional charge transport pathways, which enhance the efficiency of charge separation. This study provides insights into the dynamics of photogenerated carriers at interfaces modulated by oxygen vacancies, contributing to the development of efficient S-scheme photocatalysts.

关键词： S-scheme heterojunction Oxygen vacancy Photodegradation

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Synergistic activation of peroxymonosulfate by highly dispersed iron-based sulfur-nitrogen co-doped porous carbon for bisphenol a removal: mechanistic insights and selective oxidation

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RSC ADVANCES 2025年第6期15卷 4356-4368页

作者： Sun, Yu Zhang, Chuning Jia, Yan Zhang, Yalei Fan, Jianwei Tongji Univ Shanghai Inst Pollut Control & Ecol Secur Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China

Efficient and pervasive solutions are urgently needed to mitigate pollution from emerging contaminants in aquatic environments. Activation of peroxymonosulfate (PMS) is commonly employed to remove refractory organic pollutants from water. Herein, we synthesized sulfur-nitrogen co-doped porous carbon materials loaded with highly dispersed iron species (FeSNC) using template-assisted and ligand site construction methods. The uniform doping of N, S, and Fe in the carbon substrate, along with their synergistic effects, significantly enhanced catalytic activity by creating a high degree of defects in the catalyst (ID/IG = 1.47). This enhancement facilitated efficient removal of BPA, achieving an apparent rate constant of up to 2.83 min-1, which was 30 times higher than that of SNC and 6 times higher than that of FeNC. The FeSNC/PMS system demonstrated robust catalytic stability across the pH 3-9 range, and showed minimal sensitivity to environmental factors like the aqueous matrix, with low iron ion dissolution (<0.01 mg L-1) and certain reusability. Mechanistic investigations employing quenching experiments, EPR tests, probe experiments, and electrochemical tests elucidated that the system catalyzed the degradation of BPA via two non-radical pathways: high-valent iron oxidation and singlet oxygen pathways. Additionally, the system further exhibits selective degradation of electron-rich organics (e.g., 4-chlorophenol, sulfamethoxazole, ofloxacin, etc.).

关键词： Rate constants

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Broadening environmental research in the era of accurate protein structure determination and predictions

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Frontiers of Environmental Science & Engineering 2024年第7期18卷 169-178页

作者： Mingda Zhou Tong Wang Ke Xu Han Wang Zibin Li Wei-xian Zhang Yayi Wang State Key Laboratory of Pollution Control and Resources Reuse Shanghai Institute of Pollution Control and Ecological SecurityCollege of Environmental Science and EngineeringTongji UniversityShanghai 200092China Translational Research Institute of Brain and Brain-Like Intelligence Shanghai Fourth People's HospitalSchool of MedicineTongji UniversityShanghai 200434China

The deep-learning protein structure prediction method AlphaFold2 has garnered enormous attention beyond the realm of structural biology,for its groundbreaking contribution to solving the"protein foiding problem"In this perspective,we explore the connection between protein structure studies and environmental research,delving into the potential for addressing specific environmental *** are promising for environmental applications because of the functional diversity endowed by their structural ***,structural studies on proteins with environmental significance remain ***,we present the opportunity to study proteins by advancing experimental determination and deep-learning prediction ***,the latest progress in environmental research via cryogenic electron microscopy is *** allows us to determine the structure of protein complexes in their native state within cells at molecular resolution,revealing environmentally-associated structural *** the remarkable advancements in computational power and experimental resolution,the study of protein structure and dynamics has reached unprecedented depth and *** advancements will undoubtedly accelerate the establishment of comprehensive environmental protein structural and functional *** opportunities for protein engineering exist to enable innovative solutions for environmental applications,such as the degradation of persistent contaminants,and the recovery of valuable metals as well as rare earth elements.

关键词： Environmental proteins Protein structure Cryogenic electron microscopy Protein structure prediction Protein engineering Artificial Intelligence

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Synergistic promotion of particulate matter reduction and production performance via adjusting electrochemical reactions in the zinc electrolysis industry

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Frontiers of Environmental Science & Engineering 2024年第1期18卷 23-33页

作者： Zizhen Ma Jingkun Jiang Lei Duan Jianguo Deng Fuyuan Xu Zehui Li Linhua Jiang Ning Duan School of Environmental and Municipal Engineering Qingdao University of TechnologyQingdao 266520China State Key Joint Laboratory of Environmental Simulation and Pollution Control School of the EnvironmentTsinghua UniversityBeijing 100084China State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China School of Physics Peking UniversityBeijing 100871China

Heavy particulate matter (PM) pollution and high energy consumption are the bottlenecks of hydrometallurgy, especially in the electrolysis process. Therefore, an urgent need is to explore PM reduction methods with production performance co-benefits. This study presents three PM reduction methods based on controlling operating parameters, i.e., lowering electrolyte temperature, H2SO4 concentration, and current density of the cathode. The optimized conditions were also investigated using the response surface methodology to balance the PM reduction effect and Zn production. The results showed that lowering electrolyte temperature is the most efficient, with an 89.0% reduction in the PM generation flux (GFPM). Reducing H2SO4 concentration led to the minimum side effects on the current efficiency of Zn deposition (CEZn) or power consumption (PC). With the premise of non-deteriorating CEZn and PC, GFPM can be reduced by 86.3% at the optimal condition (electrolyte temperature = 295 K, H2SO4 = 110 g/L, current density = 373 A/m^(2)). In addition, the reduction mechanism was elucidated by comprehensively analyzing bubble characteristics, electrochemical reactions, and surface tension. Results showed that lower electrolyte temperature inhibited the oxygen evolution reaction (OER) and compressed gas volume. Lower H2SO4 concentration inhibited the hydrogen evolution reaction (HER) and reduced electrolyte surface tension. Lower current density inhibited both OER and HER by decreasing the reaction current. The inhibited gas evolutions reduced the microbubbles’ number and size, thereby reducing GFPM. These results may provide energy-efficient PM reduction methods and theoretical hints of exploring cleaner PM reduction approaches for industrial electrolysis.

关键词： Zinc electrolysis Particulate matter Energy consumption Operating parameters Bubble characteristic Electrochemical reaction

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Degradation of iopamidol in the permanganate/sulfite process:Evolution of iodine species and effect on the subsequent formation of disinfection by-products

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Journal of Environmental Sciences 2024年第1期135卷 345-352页

作者： Yimin Lin Hongyu Dong Yating Zhu Gongming Zhou Junlian Qiao Xiaohong Guan State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Department of Environmental Science School of Ecological and Environmental SciencesEast China Normal UniversityShanghai 200241China

Permanganate/sulfite(Mn(VII)/S(IV))process is a promising pre-oxidation technology for sequestering the emerging organic contaminants in drinking water treatment ***(IPM),a representative of iodinated X-ray contrast media,has been widely detected in water sources and has the risk of forming iodinated disinfection byproducts(I-DBPs)in water treatment *** this study,we investigated the evolution of iodine species during the IPM degradation by the Mn(VII)/S(IV)process and its effect on the subsequent formation of I-DBPs during chlorination at pH 7.0 and *** could be effectively degraded in the Mn(VII)/S(IV)process at environmentally relevant pH(pH 7.0 and 8.0).The results of quenching and competitive oxidation kinetic experiments revealed that SO^(·-)_(4)was the major reactive oxidizing species contributing to the degradation of IPM whereas the contributions of HO·and reactive manganese species were negligible in the Mn(VII)/S(IV)process.I–and IO–3were generated while no HOI was detected during the degradation of IPM in the Mn(VII)/S(IV)*** effects of IPM oxidation by Mn(VII)/S(IV)on the subsequent formation of chlorinated disinfection by-products(Cl-DBPs)during chlorination were related to the category of *** pre-oxidation of IPM by Mn(VII)/S(IV)resulted in the generation of I-DBPs during the disinfection process although no I-DBPs were detected if no pre-oxidation was *** finding of this study suggested that attention should be paid to the toxicity of DBPs when water containing iodinated organic contaminants is treated by Mn(VII)/S(IV)process or other pre-oxidation technologies.

关键词： Permanganate/sulfite Iopamidol Sulfate radical Iodinated disinfection byproducts Pre-oxidation

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A novel approach to assessing the anaerobic bio-accessibility of straw using fractal dimension

Waste Management Bulletin

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Waste Management Bulletin 2024年第2期2卷 208-212页

作者： Hua, Yu Yan, Wenjing Li, Dongni Ma, Yike Yang, Yunyun Li, Junxian Chen, Shuxian Dai, Xiaohu State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and Engineering Tongji University Shanghai 200092 China

Traditional methods for evaluating the bioconversion capacity of organic solid waste are known for time-consuming property and often exhibit low prediction accuracy. However, leveraging fractal dimensions offers a more precise characterization of the complexity, irregularity, and spatial structure of organic solid waste. In this study, a novel and efficient method for evaluating the bio-accessibility of straw's anaerobic transformation, based on fractal dimensions, was introduced. To comprehensively compare the structural differences, this research encompasses the measurement of nine different varieties of straw under ten distinct pretreatment conditions. The regression sum of squares for these correlations consistently exceeds 0.83, highlighting the robustness of our findings. The results unequivocally demonstrate the close relationship between the fractal dimension and the structural characteristics of straw. This relationship underscores the utility of fractal dimension analysis as a reliable tool for evaluating the anaerobic bio-accessibility of organic solid waste. © 2024 The Authors

关键词： Fractal geometry Internal structural characteristics Organic solid waste Prediction method

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Simultaneous Degradation, Dehalogenation, and Detoxification of Halogenated Antibiotics by Carbon Dioxide Radical Anions

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Engineering 2024年第6期37卷 78-86页

作者： Yanzhou Ding Xia Yu Shuguang Lyu Huajun Zhen Wentao Zhao Cheng Peng Jiaxi Wang Yiwen Zhu Chengfei Zhu Lei Zhou Qian Sui State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process School of Resources and Environmental EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Academy of Environmental Sciences Shanghai 200233China

Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of *** moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification *** address these limitations of AOPs,advanced reduction processes(ARPs)have been ***,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated *** results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of *** detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based *** identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real ***,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halog

关键词： Carbon dioxide radical anions Advanced reduction processes Halogenated antibiotics Dehalogenation Detoxification

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Strategies for optimizing the efficiency and selectivity of photocatalytic aqueous CO2 reduction: Catalyst design and operating conditions

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NANO ENERGY 2025年 133卷

作者： Li, Danping Wang, Kaichong Li, Jia Li, Zibin Wang, Han Wang, Yayi Tongji Univ Shanghai Inst Pollut Control & Ecol Secur Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Siping Rd Shanghai 200092 Peoples R China

Photocatalytic carbon dioxide (CO2) reduction (CO2R) technology towards carbon neutrality is a green and sustainable method to produce carbonous feedstocks (e.g., methane, ethanol, acetic acid). However, the relatively low CO2R efficiency and unsatisfactory selectivity towards target products hinder its scale-up implementation. Photocatalysts and operating conditions are pivotal in tuning the catalytic environment and governing CO2R activity. Herein, the photocatalytic CO2R mechanism and conversion pathways for main C1/C2/ C3 products are elaborated. Then, the recent advances in promoting CO2 photoreduction efficiency and selectivity are summarized and discussed, paying special attention to the catalyst design approaches (defect design and interfacing engineering), as well as the operating conditions (e.g., light intensity and wavelength, pH, CO2 pressure/concentration, solvent volume, dissolved oxygen, and coexisting ions) which directly affect the catalytic environment. Future researches on photocatalytic CO2R are proposed in terms of efficient catalyst design, intrinsic transformation mechanism, and sustainable application-oriented CO2R technologies. The insights obtained will advance our mechanistic understanding of regulating CO2R pathways, and help drive the adoption of sustainable and highly efficient strategies for producing desired products.

关键词： Photocatalytic CO 2 reduction Aqueous phase Catalyst design Operating conditions Pathways

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Comprehensive review of microbial production of medium-chain fatty acids from waste activated sludge and enhancement strategy

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BIORESOURCE TECHNOLOGY 2024年 402卷 130782页

作者： Gu, Xin Sun, Jing Wang, Tong Li, Jia Wang, Han Wang, Jialin Wang, Yayi Tongji Univ Shanghai Inst Pollut Control & Ecol Secur Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China

Microbial production of versatile applicability medium -chain fatty acids (MCFAs) (C6 -C10) from waste activated sludge (WAS) provides a pioneering approach for wastewater treatment plants (WWTPs) to achieve carbon recovery. Mounting studies emerged endeavored to promote the MCFAs production from WAS while struggling with limited MCFAs production and selectivity. Herein, this review covers comprehensive introduction of the transformation process from WAS to MCFAs and elaborates the mechanisms for unsatisfactory MCFAs production. The enhancement strategies for biotransformation of WAS to MCFAs was presented. Especially, the robust performance of iron -based materials is highlighted. Furthermore, knowledge gaps are identified to outline future research directions. Recycling MCFAs from WAS presents a promising option for future WAS treatment, with iron -based materials emerging as a key regulatory strategy in advancing the application of WAS-to-MCFAs biotechnology. This review will advance the understanding of MCFAs recovery from WAS and promote sustainable resource management in WWTPs.

关键词： Medium chain carboxylate Sludge hydrolysis Chain elongation Iron -based materials Electron transfer efficiency

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New insights into FeS/persulfate system for tetracycline elimination:Iron valence,homogeneous-heterogeneous reactions and degradation pathways

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Journal of Environmental Sciences 2022年第2期34卷 48-58页

作者： Jinhong Fan Ying Cai Shihao Shen Lin Gu State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

In this study,complete tetracycline(TTC)and above 50%of total organic carbon(TOC)were removed by Fe S/PS after 30 min under optimized *** free radicals and high-valent iron ions were identified to generate in the process,the apparent similarity between intermediate products of Fe S/PS,Fe/PS,and UV/PS systems demonstrated that the degradation of TTC was due to sulfate radicals(SO_(4)·^(-))and hydroxyl radicals(·OH).Based on the reaction between free radicals and organic matter,we speculated that TTC in the Fe S/PS system was decomposed and mineralized by dehydration,dehydrogenation,hydroxyl addition,demethylation,substitution,E-transfer,and ***,a new understanding of Fe S-mediated PS activation based on stoichiometry and kinetic analysis showed that there were both homogeneous and heterogeneous reactions that occurred in the entire ***,due to the effect of p H on the dissolution of iron ions,the homogeneous reaction became the principal process with iron ions concentration exceeding 1.35 mg/*** work provides a theoretical basis for the study of the degradation of TTC-containing wastewater by the iron-based advanced oxidation process.

关键词： Tetracycline Persulfate activation Iron valence Homogeneous-heterogeneous reactions Degradation pathways

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