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Ultrasonic enhancement of persulfate oxidation system governs emerging pollutants decontamination

Green Energy & Environment 2024年第11期9卷 1666-1678页

作者： Yanpan Li Yanbo Zhou Yi Zhou National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical ProcessEast China University of Science and Technology130 Meilong RoadShanghai200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and Technology130 Meilong RoadShanghai200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

Emerging contaminants (ECs) are widely present in aquatic environments, posing potential risks to both ecosystems and human health. Theultrasound-assisted persulfate oxidation process has attracted considerable attention in the degradation of ECs due to its ability to generate bothsulfate radicals and cavitation effects, enhancing degradation effects. In this paper, the principle of ultrasonic synergistic Fenton-like oxidationsystem for degrading organic pollutants was reviewed, divided into homogeneous system, non-homogeneous system, and single-atom system toexplore the synergistic effect of ultrasound-enhanced persulfate technology in three aspects, and the effects of environmental factors such asultrasonic frequency and power, system pH, temperature, and initial oxidant concentration on the system's decontamination performance werediscussed. Finally, future research on ultrasonically activated persulfate technology is summarized and prospected.

关键词： Ultrasound Persulfate Emerging contaminants Reaction mechanism Synergistic effects

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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering&PharmacyWuhan Institute of TechnologyWuhan 430205HubeiChina Key Laboratory of Pesticide&Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079HubeiChina College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108FujianChina

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction(OER).Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER ***,most of them undergo incomplete reconstruction with limited thickness of reconstruction layer,leading to low component utilization and arduous exploration of real catalytic ***,we identify the dynamic behaviors in complete reconstruction of Co-based complexes during *** hollow phytic acid(PA)cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability,in favor of the fast and complete reconstruction.A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co(Fe)(OH)xand subsequent potential-driven oxidation to Co(Fe)*** obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm^(-2)and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER *** work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

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Green innovation unleashed:Harnessing tungsten-based nanomaterials for catalyzing solar-driven carbon dioxide conversion

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Chinese chemical Letters 2025年第2期36卷 108-117页

作者： Weidan Meng Yanbo Zhou Yi Zhou State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and TechnologyShanghai 200237China National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery East China University of Science and TechnologyShanghai 200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai 200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Carbon dioxide photocatalytic reduction (CO_(2)-PR) is an efficient method for controlling CO_(2)emissions and generating cleaner energy while mitigating global *** oxides (WxOy) have attracted considerable attention for CO_(2)-PR due to their excellent spectral ***,comprehensive reviews are lacking on the use of WxOyfor CO_(2)-***,this review provides a detailed summary of t research progress made with WxOy-based catalysts in CO_(2)-*** also explains the fundamental principles of CO_(2)-PR and evaluates key performance indicators that affect the activity of WxOy-based photocatalysts,including yield,selectivity,stability,and apparent quantum ***,this review explores opportunities for synthesizing high-performance WxOy-based photocatalysts and highlights their potential for the green preparation of C1/C2 products through CO_(2)-*** innovative strategies aim to address the challenges and pressures associated with energy and environmental issues,particularly by enhancing artificial photosynthesis efficiency.

关键词： Carbon dioxide photoreduction Tungsten-based nanocatalyst Mechanism Performance evaluation Selectivity

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High concentration of Ti^(3+)in C-TiO_(x)nanosheets boosting efficient photodegradation

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Science China(Technological Sciences) 2025年第3期68卷 156-166页

作者： Chongbei WU Xuan LI Haibin WANG Jiaxin TANG Shuai WEI Yuanyuan WU Aobing WANG Jizhou JIANG Hebei Key Laboratory of Man-machine Environmental Thermal Control Technology and Equipment Hebei Vocational University of Technology and EngineeringXingtai054000China School of Materials Science and Engineering Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationWuhan Institute of TechnologyWuhan430205China

Semiconductor photocatalysis holds significant promise for addressing dye-pollution in ***,the efficiency of photocatalytic water purification is constrained by the weak light absorption capacity and low active site distribution of *** a bottom-up approach,carbon-doped TiO_(x)(C-TiO_(x))nanosheets with high concentrations of Ti^(3+)active sites were fabricated by etching the Al element in Ti_(3)Ai C_(2)with H_(2)O_(2).Experimental evidence demonstrates that the optimal C-TiO_(x)nanosheets exhibit high activity for the photocatalytic degradation of methylene blue,achieving a degradation rate of 100%within 50 *** introduction of carbon into the C-TiO_(x)nanosheets induces a red shift in the absorption edge,boosting the migration of photo-generated charge ***,there is a significant correlation between the concentration of Ti^(3+)active sites and the density of oxygen vacancies in the C-TiO_(x)nanosheets,which synergistically influence the photocatalytic degradation performance of MB dye wastewater.

关键词： bottom-up strategies C-TiO_(x)nanosheets high-concentrations Ti^(3+) photocatalytic degradation

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Efficient photocatalytic NADH regeneration with Rh-loaded Z-scheme mediator-free system

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Chinese chemical Letters 2024年第2期35卷 496-500页

作者： Yi Zhou Yiling He Ming Gao Ningkai Ding Juying Lei Yanbo Zhou State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and TechnologyShanghai 200237China National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery East China University of Science and TechnologyShanghai 200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai 200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Nicotinamide adenine dinucleotide(NADH)regeneration is necessary for the sustainable application of enzymatic *** Rh-based complex[Cp^(*)Rh(bpy)(H)]+has been widely used as an important mediator in NADH regeneration systems,but it is limited by complexity and high ***,a Z-scheme was constructed by loading Rh onto carbon nitride nanosheets/carbon nitride quantum dots(CN-CNQD).The resultant catalyst achieved a high yield of NADH in a mediator-free(M-free)system of 0.283 mmol L^(−1) g^(−1) min^(−1),which is 5.29 times that of pure *** enzyme introduction experiments confirmed that the enzyme active product 1,4-NADH could reach 34.21%selectivity in the M-free *** research revealed that the heterojunction between CNs and CNQDs improved the NADH regeneration activity in the traditional M-involved system,while Rh loading was proved to optimize the yield and selectivity of 1,4-NADH in M-free *** immobilized Rh shows more competitiveness than[Cp^(*)Rh(bpy)(H)]^(+).This study contributes to the construction of an M-free system for further application in greener,lower-cost enzymatic processes.

关键词： Photocatalysis NADH regeneration Mediator-free Carbon nitride Z-scheme

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Unveiling the geometric site dependent activity of spinel Co_(3)O_(4)for electrocatalytic chlorine evolution reaction

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Journal of Energy Chemistry 2024年第5期92卷 95-103页

作者： Linke Cai Yao Liu Jingfang Zhang Qiqi Jia Jiacheng Guan Hongwei Sun Yu Yu Yi Huang Key Laboratory of Pesticide&Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079HubeiChina Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering&PharmacyWuhan Institute of TechnologyWuhan 430205HubeiChina College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108FujianChina School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601AnhuiChina

Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost ***,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the Co_(Oh) site acts as the main active site for CER in spinel Co_(3)O_(4),which shows better Cl^(-)adsorption and more moderate intermediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condition at applied *** by above findings,the oxygen vacancies were further introduced into the Co_(3)O_(4) to precisely manipulate the electronic configuration of Co_(Oh) to boost Cl^(-)adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity *** work figures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.

关键词： Chlorine evolution reaction Geometry effects Active chlorine Electronic configuration optimization Spinel oxides

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Recent advances in heterogeneous catalysis of solar-driven carbon dioxide conversion

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Journal of Environmental Sciences 2024年第6期140卷 165-182页

作者： Jun Xu Farzaneh Arabpour Roghabadi Ying Luo Vahid Ahmadi Qian Wang Zheng Wang Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China College of Chemistry and Chemical Engineering Henan Polytechnic UniversityJiaozuoHenan 454000China Department of Process Engineering Faculty of Chemical EngineeringTarbiat Modares UniversityTehranIran Optoelectronics and Nanophotonics Research Group Faculty of Electrical and Computer EngineeringTarbiat Modares UniversityTehranIran Graduate School of Engineering Nagoya UniversityFuro-choChikusa-kuNagoya 464-8603Japan

Solar-driven carbon dioxide(CO_(2))conversion including photocatalytic(PC),photoelectrochemical(PEC),photovoltaic plus electrochemical(PV/EC)systems,offers a renewable and scalable way to produce fuels and high-value chemicals for environment and energy *** review summarizes the basic fundament and the recent advances in the field of solar-driven CO_(2)*** the visible-light absorption is an important strategy to improve solar energy conversion *** separation and migration of photogenerated charges carriers to surface sites and the surface catalytic processes also determine the photocatalytic *** engineering including co-catalyst loading,defect engineering,morphology control,surface modification,surface phase junction,and Z-scheme photocatalytic system construction,have become fundamental strategies to obtain high-efficiency *** to photocatalysis,these strategies have been applied to improve the conversion efficiency and Faradaic efficiency of typical PEC *** PV/EC systems,the electrode surface structure and morphology,electrolyte effects,and mass transport conditions affect the activity and selectivity of electrochemical CO_(2)***,the challenges and prospects are addressed for the development of solar-driven CO_(2)conversion system with high energy conversion efficiency,high product selectivity and stability.

关键词： Solar-driven CO_(2)reduction Photocatalytic system Photoelectrochemical system Photovoltaic plus electrochemical system Surface/interface engineering

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Review on electrochemical carbon dioxide capture and transformation with bipolar membranes

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Chinese chemical Letters 2023年第8期34卷 114-129页

作者： Jinyun Xu Guoqiang Zhong Minjing Li Di Zhao Yu Sun Xudong Hu Jiefang Sun Xiaoyun Li Wenju Zhu Ming Li Ziqi Zhang Yu Zhang Liping Zhao Chunming Zheng Xiaohong Sun School of Chemical Engineering Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining TechnologyMinistry of EducationTianjin UniversityTianjin 300072China Beijing Key Laboratory of Diagnostic and Traceability Technologies for Food poisoning Beijing Center for Disease Prevention and ControlBeijing 100013China Advanced Materials Research Laboratory CNOOC Tianjin Chemical Research and Design InstituteTianjin 300131China

Anthropogenic carbon dioxide(CO_(2))emission from the combustion of fossil fuels aggravates the global greenhouse *** implementation of CO_(2)capture and transformation technologies have recently received great attention for providing a pathway in dealing with global climate *** these technologies,electrochemical CO_(2)capture technology has attracted wide attention because of its environmental friendliness and flexible operating *** membranes(BPMs)are considered as one of the key components in electrochemical devices,especially for electrochemical CO_(2)reduction and electrodialysis *** create an alkaline environment for CO_(2)capture and a stable pH environment for electrocatalysis on a single *** key to CO_(2)capture in these devices is to understand the water dissociation mechanism occurring in BPMs,which could be used for optimizing the operating conditions for CO_(2)capture and *** this paper,the references and technologies of electrochemical CO_(2)capture based on BPMs are reviewed in detail,thus the challenges and opportunities are also discussed for the development of more efficient,sustainable and practical CO_(2)capture and transformation based on BPMs.

关键词： Bipolar membranes Carbon dioxide Electrochemical capture Transformation CO_(2)reduction Electrodialysis devices Water dissociation

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In-situ synthesis of N, S co-doped hollow carbon microspheres for efficient catalytic oxidation of organic contaminants

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Chinese chemical Letters 2022年第3期33卷 1298-1302页

作者： Yongbing Xie Ya Liu Yujie Yao Yanchun Shi Binran Zhao Yuxian Wang State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization Panzhihua 617000China CAS Key Laboratory of Green Process&Engineering Beijing Engineering Research Center of Process Pollution ControlInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China State Key Laboratory of Heavy Oil Processing State Key Laboratory of Petroleum Pollution ControlChina University of Petroleum-BeijingBeijing 102249China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia School of Chemical Engineering Northwest UniversityXi'an 710069China

Metal-free heteroatom doped nanocarbons are promising alternatives to the metal-based materials in catalytic ozonation for destruction of aqueous organic contaminants. In this study, N, S co-doped hollow carbon microspheres (NSCs) were synthesized from the polymerization products during persulfate wet air oxidation of benzothiazole. The contents of doped N and S as well as the structural stability were maneuvered by adjusting the subsequent N_(2)-annealing temperature. Compared with the prevailing single-walled carbon nanotubes, the N_(2)-annealed NSCs demonstrated a higher catalytic ozonation activity for benzimidazole degradation. According to the quantitative structure-activity relationship (QSAR) analysis, the synergistic effect between the graphitic N and the thiophene-S which redistributed the charge distribution of the carbon basal plane contributed to the activity enhancement of the N_(2)-annealed NSCs. Additionally, the hollow structure within the microspheres served as the microreactor to boost the mass transfer and reaction kinetics via the nanoconfinement effects. Quenching and electron paramagnetic resonance (EPR) tests revealed that benzimidazole degradation was dominated by the produced singlet oxygen (^(1)O_(2)) species, while hydroxyl radicals (^(·)OH) were also generated and participated. This study puts forward a novel strategy for synthesis of heteroatom-doped nanocarbons and sheds a light on the relationship between the active sites on the doped nanocarbons and the catalytic performance.

关键词： Metal-free catalysis Hollow carbon microspheres N,S co-doping Catalytic ozonation Singlet oxygen(1O_(2))

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Characterization strategy of polymeric transition metal species transformation for high-purity metal recovery

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Green chemical Engineering 2021年第3期2卷 309-316页

作者： Jiawei Wen Yan Wu Shujie Lin Pengge Ning Beijing Engineering Research Center of Process Pollution Control Institute of Process EngineeringInnovation Academy for Green ManufactureChinese Academy of SciencesBeijing100190China School of Chemical Engineering and Technology Xi'an Jiaotong University28 Xianning West RoadXi'an710049China Collaborative Innovation Center of Chemical Science and Engineering Tianjin300072China

The aqueous metal species with similar chemical properties are usually extracted together,limiting deep separation for high-purity ***,rare attention has been paid to metal speciation characterization and transformation during ***,the hydrolysis evolution of polymeric metal species was investigated systematically by electrospray ionization time-of-flight mass spectrometry(ESI-TOF-MS).The transformation evolutions were visualized with respect to characteristic vanadium species(V_(1),V_(2),V_(3),V_(4) and V_(10)),chromium species(Cr_(1) and Cr_(2)),tungsten(W_(1),W_(2),W_(4),W_(6) and W_(10))and molybdenum(Mo_(1),Mo_(2) and Mo_(4))*** key characteristics(such as specfic pHs and concentrations)for speciation variation were *** polymerization behavior of several transition metals can be semiquantitative characterized by this *** sufficient speciation transformation provides a solid base for metal speciation chemistry,and guides further development of high-purity metal recovery.

关键词： Metal ion speciation WPPC Vanadium recovery Polymerization behavior ESI-TOF-MS

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