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key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge Meiling Xiao Changpeng Liu Wei Xing State key laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province key laboratory of Low Carbon Chemical Power Sources Changchun 130022China State key laboratory of Rare Earth resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron *** hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of ***,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic *** we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal *** demonstrate that the conductivity of catalysts greatly affects the overall catalytic *** further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to *** and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing *** results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.

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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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Reactive Transport process of Earthquake-induced Hydrochemical Changes in Guanding Thermal Spring,Western Sichuan,China

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Acta Geologica Sinica(English Edition) 2024年第1期98卷 241-249页

作者： NA Jin JIANG Xue SHI Zheming CHEN Yanmei Hubei key laboratory of Petroleum Geochemistry and Environment(Yangtze University) Wuhan 430100China School of Environmental Studies China University of GeosciencesWuhan 430074China School of Water resources and Environment China University of GeosciencesBeijing 100083China State key laboratory of Water resource Protection and Utilization in Coal Mining Beijing 100000China

Earthquake-related hydrochemical changes in thermal springs have been widely observed;however,quantitative modeling of the reactive transport process is *** the present study,we apply reactive transport simulation to capture the hydrochemical responses in a thermal spring following the Wenchuan Ms 8.0 and Lushan Ms 7.0 *** first constrain deep reservoir geothermal fluid compositions and temperature by multicomponent geothermometry,and then a reactive geochemical transport model is constructed to reproduce the hydrochemical evolution *** results show that the recharge from the shallow aquifer increases gradually until it reaches a peak because of the permeability enhancement caused by the Lushan earthquake,which may be the mechanism to explain the earthquake-related hydrochemical *** contrast to the postseismic effect of the Wenchuan earthquake,the chemical evolution can be considered as hydrochemical anomalies related to the Lushan *** study proves that the efficient simulation of reactive transport processes is useful for investigating earthquake-related signals in hydrochemical time series.

关键词： earthquake hydrochemical changes reactive geochemical transport model Kangding area

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Controllable surface reconstruction of copper foam for electrooxidation of benzyl alcohol integrated with pure hydrogen production

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SmartMat 2024年第1期5卷 147-157页

作者： Yingnan Han Chang Yu Hongling Huang Qianbing Wei Junting Dong Lin Chen Jieshan Qiu State key Lab of Fine Chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalianChina State key laboratory of Chemical resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijingChina

Electrocatalytic water splitting that is coupled with electrocatalytic chemical oxidation is considered as one of the promising methods for efficiently obtaining hydrogen energy and fine ***,we focus on an electrochemical redox activation strategy to rationally manipulate the microstructure and surface valence states of copper foam(CF)and boost the corresponding performance towards electrocatalytic benzyl alcohol oxidation(EBA),accompanied by the efficient hydrogen ***,the Cu(II)‐dominated species are gradually formed on the CF surface with the dissolution and redeposition of copper in the suitable potential *** new species containing Cu2O,CuO,and Cu(OH)2 during surface reconstruction process of the CF were confirmed by multiple characterization *** 220‐cycled activation(CF‐220),the activated CF achieves an increase of current density for EBA in anode from 9.5 for the original CF to 29.3 mmol/cm2,while the pure hydrogen yield increases threefold than that of the original CF at 1.5 *** produced new species can endow the CF‐220 with abundant acidity sites,which can enhance the adsorption toward Lewis‐basicity benzyl alcohol,confirmed by NH3‐temperature‐programmed *** situ Raman result further reveals that the as‐produced CuO,Cu(OH)2,and Cu(OH)42−are the main active species toward the EBA process.

关键词： benzyl alcohol copper electrochemical oxidation Lewis acid surface reconstruction

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太阳能诱导选择性分离和回收失活空气净化催化剂中的贵金属（英文）

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Science Bulletin 2024年第15期 2379-2386页

作者：伍美军陈瑶国振鹏王心茹张涵云张婷关舒会卞振锋 Ministry of Education key laboratory of resource Chemistry and Shanghai key laboratory of Rare Earth Functional Materials Shanghai Normal University Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University Shanghai YK Pao School

The mitigation of environmental and energy crises could be advanced by reclaiming platinum group precious metals(PGMs) from decommissioned air purification catalysts. However, the complexity of catalyst composition and the high chemical inertness of PGMs significantly impede this process. Consequently,recovering PGMs from used industrial catalysts is crucial and challenging. This study delves into an environmentally friendly approach to selectively recover PGMs from commercial air purifiers using photocatalytic redox technology. Our investigation focuses on devising a comprehensive strategy for treating three-way catalysts employed in automotive exhaust treatment. By meticulously pretreating and modifying reaction conditions, we achieved noteworthy results, completely dissolving and separating rhodium(Rh), palladium(Pd), and platinum(Pt) within a 12-h time frame. Importantly, the solubility selectivity persists despite the remarkably similar physicochemical properties of Rh, Pd, and Pt. To bolster the environmental sustainability of our method, we harness sunlight as the energy source to activate the photocatalysts, facilitating the complete dissolution of precious metals under natural light irradiation. This ecofriendly recovery approach demonstrated on commercial air purifiers, exhibits promise for broader application to a diverse range of deactivated air purification catalysts, potentially enabling implementation on a large scale.

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MXenes/CNTs-based hybrids:Fabrications,mechanisms,and modification strategies for energy and environmental applications

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Nano Research 2024年第5期17卷 3429-3454页

作者： Jizhou Jiang Fangyi Li Lei Ding Chengxun Zhang Arramel Xin Li School of Environmental Ecology and Biological Engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Nano Center Indonesia Jl.PUSPIPTEK Tangerang SelatanBanten 15314Indonesia Institute of Biomass Engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

Emerging two-dimensional(2D)layered metal carbide and nitride materials,commonly termed MXenes,are increasingly recognized for their applications across diverse fields such as energy,environment,and *** the past few years,MXenes/carbon nanotubes(CNTs)-based hybrids have attracted extensive attention as an important catalyst in energy and environmental fields,due to their superior multifunctions and mechanical *** review aims to address the fabrication strategies,the identification of the enhancement mechanisms,and recent progress regarding the design and modification of MXenes/CNTs-based hybrids.A myriad of fabrication techniques have been systematically summarized,including mechanical mixing,spray drying,three-dimensional(3D)printing,self-assembly/in-situ growth,freeze drying,templating,hydrothermal methods,chemical vapor deposition(CVD),and ***,the identification of the enhancement mechanisms was thoroughly discussed from the two dimensions of theoretical simulations and in-situ ***,the recent advancements in profound applications of MXenes/CNTs-based hybrids have also been carefully revealed,including energy storage devices,sensors,water purification systems,and microwave *** also underscore anticipated challenges related to their fabrication,structure,underlying mechanisms,modification approaches,and emergent ***,this review offers insights into prospective directions and the future trajectory for these promising *** is expected that this review can inspire new ideas or provide new research methods for future studies.

关键词： MXenes/carbon nanotubes(CNTs)-based hybrids fabrication applications modification strategies

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Assembling S-scheme heterojunction between basic bismuth nitrate and bismuth tungstate with promoting charges’separation for accelerated photocatalytic sulfamethazine degradation

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Journal of Materials Science & Technology 2024年第4期171卷 185-197页

作者： Wenhan Chen Meng Dai Li Xiang Shan Zhao Shuguang Wang Zuoli He Shandong key laboratory of Water Pollution Control and resource Reuse Shandong Key Laboratory of Environmental Processes and HealthSchool of Environmental Science and EngineeringShandong UniversityQingdao 266237China CEDAR Knight Cancer InstituteSchool of MedicineOregon Health and Science UniversityPortlandOR 97201United States Weihai Research Institute of Industrial Technology of Shandong University Shandong UniversityWeihai 264209China

The S-scheme heterojunction has garnered increasing attention due to its remarkable oxidation capacity and efficient separation of photogenerated *** this study,a one-pot glycerol-assisted hydrothermal process was utilized to successfully synthesize S-scheme heterojunction photocatalysts comprising basic bismuth nitrate(BBN)and bismuth tungstate(BWO).Interestingly,the BBN/BWO heterogeneous photo-catalysts exhibited the highest photocatalytic *** optimized product achieved the degradation of sulfamethazine(SMZ)within 1 h,with a kinetic constant(k)value of 0.05818 min^(−1).The degradation process was influenced significantly by·O^(2)−and h^(+)*** determine the degradation pathway of SMZ in the presence of BBN/BWO-0.6,liquid chromatography-mass spectrometry(LC-MS)analysis was performed,which revealed a decrease in the toxicity of intermediates and *** enhanced pho-tocatalytic activity can be attributed to the internal electric field(IEF)of the S-scheme heterojunction between BBN and BWO,effectively promoting the separation of photogenerated *** research presents a viable approach for developing S-scheme heterojunctions in SMZ photodegradation and other environmental applications.

关键词： Photocatalysis S-scheme Heterojunction Bi_(2)WO_(6) Sulfamethazine

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Cobalt doping amount determines dominant reactive species in peroxymonosulfate activation via porous carbon catalysts co-doped by cobalt and nitrogen

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Journal of Environmental Sciences 2024年第4期138卷 212-226页

作者： Xiang Li Limeng Wu Aiqin Zhang Shaohua Wu Yan Lin Chunping Yang key laboratory of Jiangxi Province for Persistent Pollutants Control and resources Recycle Nanchang Hangkong UniversityNanchang 330063China Academy of Environmental and resource Sciences School of Environmental Science and EngineeringGuangdong University of Petrochemical TechnologyMaoming 525000China College of Environmental Science and Engineering Hunan University and Key Laboratory of Environmental Biology and Pollution Control(Hunan University)Ministry of EducationChangsha 410082China

Switching the reaction routes in peroxymonosulfate(PMS)-based advanced oxidation processes have attracted much attention but remain ***,a series of Co-N/C catalysts with different compositions and structures were prepared by using bimetallic zeolitic imidazolate frameworks based on ZIF-8 and ZIF-67(x Zn/Co-ZIFs).Results show that Co doping amount could mediate the transformation of the activation pathway of PMS over CoN/*** Co doping amount was less than 10%,the constructed x Co-N/C/PMS system(x≤10%)was singlet oxygen-dominated reaction;however further increasing Co doping amount would lead to the generation and coexistence of sulfate radicals and high-valent cobalt,besides singlet ***,the nitrogen-coordinated Co(Co-NX)sites could serve as main catalytically active sites to generate singlet *** excess Co doping amount caused the formation of Co nanoparticles from which leached Co ions were responsible for the generation of sulfate radicals and high-valent *** to undoped N/C,Co doping could significantly enhance the catalytic *** 0.5%Co-N/C could achieve the optimum degradation(0.488 min^(-1))and mineralization abilities(78.4%)of sulfamethoxazole among the investigated Co-N/C catalysts,which was superior to most of previously reported *** addition,the application prospects of the two systems in different environmental scenarios(pH,inorganic anions and natural organic matter)were assessed and showed different degradation *** study provides a strategy to regulate the reactive species in PMS-based advanced oxidation process.

关键词： Peroxymonosulfate Sulfate radical Singlet oxygen Cobalt Zeolitic imidazolate framework Advanced oxidation process

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Hollow Ni Mo-based nitride heterojunction with super-hydrophilic/aerophobic surface for efficient urea-assisted hydrogen production

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Journal of Energy Chemistry 2024年第8期95卷 428-439,I0009页

作者： Yuying Fan Ying Gu Dongxu Wang Yanqing Jiao Aiping Wu Chungui Tian key laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080HeilongjiangChina College of Chemistry Chemical Engineering and Resource UtilizationNortheast Forestry UniversityHarbin 150040HeilongjiangChina

Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/*** design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great ***,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal *** Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the *** functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and *** virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.

关键词： Hydrogen evolution Transition metal nitrides Hollow heterojunctions Urea electrooxidation Super hydrophilic/aerophobic

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Removal of pathogenic indicator microorganisms during partial nitrification:the role of free nitrous acid

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Frontiers of Environmental Science & Engineering 2024年第3期18卷 93-102页

作者： Jiaojiao Xu Xiaotian Chen Rui Tang Jingwei Feng Shoujun Yuan Wei Wang Zhen-Hu Hu Anhui Engineering laboratory of Rural Water Environment and resource School of Civil EngineeringHefei University of TechnologyHefei 230009China Hefei 168 High School Hefei 230025China Shanghai key laboratory of Materials Protection and Advanced Materials in Electric Power Shanghai University of Electric PowerShanghai 200090China

Digested wastewater contains pathogenic microorganisms and high ammonia concentrations,which can pose a potential risk to public *** removal of pathogens and nitrogen is crucial for the post-treatment of digested *** nitrification-anammox is an energy-saving nitrogen removal *** nitrous acid(FNA),an intermediate product of partial nitrification,has the potential to inactivate ***,the efficiency and mechanisms of FNA-related inactivation in pathogens during partial nitrification remains *** this study,Enterococcus and Escherichia coli(***)were selected to investigate the efficiency and mechanisms of FNA-related inactivation in partial nitrification *** results revealed that 83%±13%and 59%±27%of *** and Enterococcus were removed,respectively,in partial nitrification process at FNA concentrations of 0.023−0.028 mg/*** the concentration of FNA increased from 0 to 0.5 mg/L,the inactivation efficiencies of *** and Enterococcus increased from 0 to 99.9%and 89.9%,*** exhibited a higher resistance to FNA attack compared to ***.3D-laser scanning microscopy(3D-LSM)and scanning electron microscopy(SEM)revealed that FNA exposure caused the surface collapse of *** and Enterococcus,as well as visible pore formation on the surface of *** cells.4',6-Diamidino-2-phenylindole dihydrochloride n-hydrate(DAPI)/propidium iodide(PI)and biomolecule leakage confirmed that inactivation of *** and Enterococcus occurred due to breakdown of cell walls and cell *** findings indicate that partial nitrification process can be used for the removal of residual pathogenic microorganisms.

关键词： Partial nitrification Free nitrous acid Pathogenic indicator microorganism Inactivation Cell structure

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