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Investigation of desiccation cracking of earthen site soils treated by enzymeinduced calcium carbonate precipitation(EICP) 认领 引用 被引量：3
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作者 Jianwei Zhang Peikun Wang +4 位作者 Yue Dong Junjie Zheng Yu Song Hanlong Liu Min Zhang 《Biogeotechnics》 2026年第3期25-35,共11页
The infiltration of groundwater and surface water is critical for the development of desiccation cracking of earthen site soils.It potentially leads to changes in the microscopic structures of pore water networks,posi... The infiltration of groundwater and surface water is critical for the development of desiccation cracking of earthen site soils.It potentially leads to changes in the microscopic structures of pore water networks,posing a threat to the stability of earthen site soils.In this study,the effects of cementation solution concentrations on water holding capacity of earthen site soils and microscopic characteristics were investigated using the methods of enzyme-induced calcium carbonate precipitation(EICP),volumetric shrinkage and suction tests under wetting-drying loadings,and microscopic tests.The microscopic characteristics regarding pore structures were used to interpret the mechanism of desiccation cracking of EICP-treated earthen site soils from the microscopic perspective.The results show that the rate of drying shrinkage and sensitivity to drying and wetting conditions of earthen site soils are notably reduced by the method of EICP.The volumetric shrinkage curves appear three-stage evolving trends.The microscopic tests show that the treated earthen site soils feature bimodal distributions of pore structures.With this regard,the uniformities of pores are significantly improved,for which large and medium pores of untreated soils are filled by the method of EICP.Small and micro pores are compressed,which reduces the potential connectivity of pores inside earthen site soils.The research outcomes can provide fundamental knowledge for improving desiccation cracking of earthen site soils by the method of EICP. 展开更多
关键词 Earthen site soil Desiccation cracking Enzyme-induced calcium carbonate precipitation(EICP) Distribution of pores
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Identification of active sites and mechanism of CO2 methanation over Ni/CeO2 catalysts 认领 引用 被引量：1
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作者 Zhaorui Zhang Zhaohui Li +5 位作者 Xiao Han Junhong Zhang Jinsheng Zhao Lingcong Li Peng Xu Ningqiang Zhang 《Journal of Rare Earths》 SCIE EI CAS CSCD 2026年第5期1490-1498,共9页
CO2 hydrogenation into methane via Sabatier reaction is an attractive process.Ceria-supported nickel(Ni/CeO2)catalysts demonstrate high activity for CO2 hydrogenation to methane,yet the nature of the active s... CO2 hydrogenation into methane via Sabatier reaction is an attractive process.Ceria-supported nickel(Ni/CeO2)catalysts demonstrate high activity for CO2 hydrogenation to methane,yet the nature of the active sites remains a topic of debate.In this work,a series of Ni/CeO2 catalysts with different dispersion of Ni species was prepared by impregnation method via adjusting loading of Ni.Turnover frequency and apparent activation energy in CO2 methanation are demonstrated to be significantly influenced by the dispersion of Ni species.Relatively large Ni nanoparticles are active sites for CO2 methanation reaction rather than highly dispersion Ni species on CeO2.Through isothermal and temperature-programmed surface reaction,and in situ/operando spectroscopies,including X-ray photoelectron spectroscopy and diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS),we unravel the coexistence of CO and HCOO-/HCO3- pathways over Ni(15)/CeO2(15 wt%Ni loading)catalyst in CO2 methanation reaction at 350℃.Those findings provide guidance for designing efficient Ni-based methanation catalysts,thereby contributing to the achievement of carbon neutrality. 展开更多
关键词 CO2methanation Ni/CeO2 Active sites Surface reaction Operando spectroscopy Rare earths
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2D nonlinear seismic response characteristics of a cross-strait seabed site considering seawater-seabed coupling effects 认领 引用
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作者 Chen Guoxing Jiang Zhijie +3 位作者 Wang Yanzhen Zhao Kai Chen Weiyun Charng-Hsein Juang 《Earthquake Engineering and Engineering Vibration》 SCIE EI CSCD 2026年第3期591-618,共28页
Existing research indicates that seismic responses in deep soft seabeds are affected by fluid-solid coupling,seabed micro-topography,soil spatial heterogeneity,and nonlinearity.To address these complexities,this study... Existing research indicates that seismic responses in deep soft seabeds are affected by fluid-solid coupling,seabed micro-topography,soil spatial heterogeneity,and nonlinearity.To address these complexities,this study develops an integrated nonlinear seismic response analysis for a cross-strait transect.The method comprehensively incorporates the strait basin geometry,detailed seabed microtopographic features,spatially varying soil properties(including S and P wave velocity structures),a nonuniform mesh layout of the transect,and appropriate artificial boundary conditions.Particular emphasis is placed on the seawater-seabed interaction,simulated via a weak coupling algorithm for fluid-solid interaction,and on the soil’s nonlinear hysteretic behavior.Numerical simulations,conducted without considering seawater effects,reveal three key findings.First,bedrock motion components near the seabed fundamental frequency show enhanced upward propagation through the soil deposits.Second,seabed microtopography exerts a more pronounced influence on vertical seafloor motions than on horizontal components.Third,a resonance-like phenomenon occurs near 2 Hz for both horizontal and vertical motion components.The complex interplay of seismic wave reflection,refraction,and interference within heterogeneous deposits generates intricate,strongly coupled amplification patterns.However,when seawater-seabed coupling is considered,significant suppression of seafloor peak accelerations is observed,especially in deepwater regions.Vertical motions exhibit more pronounced suppression within specific narrow frequency bands compared to horizontal motions.The seabed seismic responses exhibit significant higher-frequency suppression(near 4-5 Hz)and low frequency amplification(<0.5 Hz),while the resonance-like responses near 2.0 Hz for both horizontal and vertical components are diminished.Crucially,the degree of suppression or amplification of these resonance-like responses correlates positively with the seabed bedrock motion intensity. 展开更多
关键词 nonlinear seismic site response large-scale seabed site seabed micro-topography soil spatial heterogeneity fluid-solid coupling effect
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Synergistic BrФnsted and Lewis acid sites for selective catalytic valorization of isopropanol from VOC streams 认领 引用
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作者 Honghong Zhang Zhiwei Wang +5 位作者 Lu Wei Zhiquan Hou Yuxi Liu Hongxing Dai Zhenxia Zhao Jiguang Deng 《Green Energy & Environment》 SCIE EI CAS CSCD 2026年第2期545-556,共12页
Directional catalytic transformation of volatile organic compounds(VOCs)into value-added chemicals represents a more sustainable strategy than complete mineralization,as it simultaneously mitigates environmental pollu... Directional catalytic transformation of volatile organic compounds(VOCs)into value-added chemicals represents a more sustainable strategy than complete mineralization,as it simultaneously mitigates environmental pollution and reduces carbon emissions.The primary challenge in achieving multifunctional olefin production from alcohol-type VOCs is the lack of mechanistic clarity,which hinders the targeted synthesis of selective catalysts.Herein,we developed W-Ti hybrid metal oxide catalysts(WTiOx)with active Ti-O-W interfaces via a one-step hydrothermal synthesis and demonstrated their effectiveness for isopropanol conversion processes.Remarkably,WTiOx-500 achieved 99.8%isopropanol conversion and 99.3% propylene yield at 140℃,significantly outperforming TiO2(98.4% yield at 180℃)and WO3(90.5% yield at 240℃).WTiOx-500 also displayed higher thermal stability,with isopropanol conversion and propylene yield decreasing by 1.0%and 1.6% after 35 h on-stream reaction.Although impurities(e.g.,CO2,HCl,SO2)caused partial deactivation of WTiOx-500,oxygen treatment regenerated the catalyst.A series of characterization techniques indicated that the controlled calcination temperature promoted the formation of an optimal Ti-O-Winterface in WTiOx-500 through W substitution into the TiO2lattice and WO3-TiO2surface interaction,where W species effectively tuned the electronic structure.This configuration endowed WTiOx-500 with moderate acidity of BrФnsted(-OH)and Lewis(Ti4+/W6+)acid sites,which synergistically facilitated charge transfer between isopropanol and catalyst,accelerated C-O bond cleavage during dehydration.This work provides mechanistic insights into isopropanol dehydration and demonstrates a potential approach for VOC valorization. 展开更多
关键词 Brønsted/Lewis acid sites Ti-O-W interfacial sites Electronic structure VOC valorization Isopropanol conversion
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Engineering Geometric Active Sites in Cobalt Spinel Oxides for Energy and Environmental Catalysis 认领 引用
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作者 Shenning Liu Yining Ban +4 位作者 Ya Liu Jingwen Zhang Xiaoguang Duan Chunmao Chen Yuxian Wang 《Rare Metals》 SCIE EI CAS CSCD 2026年第4期5-26,共22页
Cobalt-based spinel oxides(Co3O4 and derivatives)are among the most promising transition metal oxides for electrochemical energy conversion and environmental catalysis due to their abundant active sites,structural ... Cobalt-based spinel oxides(Co3O4 and derivatives)are among the most promising transition metal oxides for electrochemical energy conversion and environmental catalysis due to their abundant active sites,structural tunability,and robust redox flexibility.However,their catalytic efficiency is often limited by ambiguities in active-site identification and insufficient control of electronic structures.This review systematically elucidates the interplay between geometric site configurations,electronic states,and catalytic performance in Co-based spinels,highlighting three key descriptors,that is,eg2 orbital occupancy,d-band center position,and Co-O covalency,as fundamental metrics for activity prediction.Based on these activity descriptors,we examine geometric-site engineering strategies including site inversion,cation substitution,defect modulation,and facet control,which precisely regulate orbital filling,spin polarization,and covalency competition to optimize catalytic activity and selectivity.Additionally,controversial results by employing these engineering strategies are critically discussed.Despite advances,challenges remain in disentangling site contributions under dynamic reaction conditions and integrating theoretical and operando insights.We conclude with an outlook on rational atomic-level design,emphasizing multidimensional descriptors as predictive tools to transition Co-based spinels from empirical optimization toward systematic catalyst development for sustainable energy and environmental technologies. 展开更多
关键词 activity descriptors co-based spinels geometric sites geometric-activity dependence site engineering strategies
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Distribution characteristics,source apportionment and risk assessment of heavy metal pollution in typical redevelopment sites in Jinshan District,Shanghai,China 认领 引用
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作者 Cheng Shen Chenyan Sha +7 位作者 Tianhao He Zhongchun Yan Xiurong Chen Kuangfei Lin Haichao Chen Jian Wu Ye Li Min Liu 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第5期197-208,共12页
As urban renewal accelerates,heavy metals(HMs)pollution resulting from industrial activities in urban areas must be considered.This study examines 36 representative redevelopment industrial sites in the Jinshan Distri... As urban renewal accelerates,heavy metals(HMs)pollution resulting from industrial activities in urban areas must be considered.This study examines 36 representative redevelopment industrial sites in the Jinshan District of Shanghai,where the concentrations of eight HMs in the soil were assessed.Based on this data,the characteristics of heavy metal concentrations and their sources in the region were investigated,followed by a risk assessment of HMs pollution.The results indicate that the soil in the study area exhibits low levels of pollution,with moderate ecological risks.Using Pearson correlation analysis and the Absolute Principal Component Score-Multiple Linear Regression(APCS-MLR)source apportionment model,the HMs were categorized into several sources:An industrial source dominated by Cu(74.84%),a traffic source dominated by Zn(67.51%),a natural source dominated by Cr and As(66.50%and 64.98%,respectively),and a mixed source.A probabilistic risk assessment was conducted using Monte Carlo simulation,which incorporates the probability distributions of various assessment parameters,thereby reducing uncertainty in the results.The findings show that the non-carcinogenic risk for all populations in the study area(children,adult females,and adult males)remains within acceptable limits.However,the carcinogenic risk proportional probabilities for these populations were found to be 48.13%,32.49%,and 11.41%,respectively,indicating a notable risk level.Uncertainty analysis results suggest that the heavy metals Cd and As exhibit high sensitivity in the model.This study provides theoretical support for the prevention and control of soil pollution during urban renewal. 展开更多
关键词 Redevelopment site Heavy metal Source apportionment Risk assessment
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Distribution and influencing factors of soil and groundwater pollution at pharmaceutical sites in China 认领 引用
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作者 Ying Hou Yi Shi +10 位作者 Weiguang Zhao Yifei Liu Nuchao Xu Hongxia Hu Haoyuan Wang Meng Yu Bochao Zhang Guizhen Hao Hongguang Zheng Juejun Yao Aizhong Ding 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第8期690-699,共10页
Owing to the rapid development of the pharmaceutical industry in China,contamination at legacy sites has become a major challenge that threatens the ecological environment and human health.Despite this growing concern... Owing to the rapid development of the pharmaceutical industry in China,contamination at legacy sites has become a major challenge that threatens the ecological environment and human health.Despite this growing concern,the distribution characteristics of contaminants at these legacy sites remain unclear.Therefore,we conducted a systematic analysis of the distribution characteristics,influencing factors,and health risks of soil and groundwater pollution at the legacy sites of 21 pharmaceutical enterprises.The results obtained identified heavy metals(As,Hg,and Pb),volatile organic compounds(VOCs)(benzene and trichloromethane),semi-volatile organic compounds(SVOCs)(benzo[a]pyrene),and inorganic salts(ammonia nitrogen and fluoride)as the major contaminants at the legacy sites.Heavy metals were primarily distributed in fill and clay layers,while the distribution of VOCs,which showed stronger vertical migration,was more diverse.Additionally,the vertical distribution pattern of the pollutants was primarily influenced by their production history,physicochemical properties,and site hydrogeological conditions.Via health risk assessment,As,Hg,and benzene were identified as major pollutants in terms of carcinogenic and non-carcinogenic risks,with the carcinogenic and non-carcinogenic(HI)risks of As(maximum value 2.97×10-3)and benzene(HI up to 10,200)significantly exceeding acceptable levels.Human exposure pathways included soil ingestion,air inhalation,and dermal contact.Overall,these findings serve as a reference for decision-making in risk identification and the development of pollution management and remediation strategies for legacy sites in the pharmaceutical industry. 展开更多
关键词 Pharmaceutical sites Soil-groundwater Vertical distribution Influencing factors Human health risks
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Dynamic coordination transformation from single-to dual-metal sites in MOFs for cascaded photoreforming of plastics into CO 认领 引用
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作者 Jian Li Zhenfa Wu +6 位作者 Xinru Zhang Tongan Yan Jin Luo Wenjuan Xue Zhaolin Lv Hongliang Huang Chongli Zhong 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第5期314-323,共10页
Building on the success of catalytic single-metal sites(SMSs)in various model reaction systems,dual-metal sites(DMSs)could provide further breakthrough on catalysing complex reactions especially for those involving mu... Building on the success of catalytic single-metal sites(SMSs)in various model reaction systems,dual-metal sites(DMSs)could provide further breakthrough on catalysing complex reactions especially for those involving multiple cascading steps.Specifically,photocatalytic waste plastic conversion requires bond cleavage into small molecules followed by site-dependent transformations,where DMSs photocatalysts can,in principle,be highly active and selective through efficient charge separation and dual-site synergy.However,related studies remain rare since difficulty on efficient waste plastic photodegradation usually hinders subsequent catalytic conversion.Herein,we report for the first time that dual-metal sites are developed in a two-dimensional metal-organic framework(MOF)(Cu2-DMSs/MOF)derived from single-metal sites in bulk MOF(Cu1-SMSs/MOF)via dynamic coordination-driven transformation.The Cu2-DMSs/MOF catalyst exhibits enhanced photocatalytic performance without sacrificial agents,catalysing the cascading polyethylene-to-CO2 and CO2-to-CO reactions in one step.The polyethylene-to-CO2 degradation rate is 2.32 mmol·g-1·h-1 and the subsequent CO2-to-CO conversion proceeds at 0.29 mmol·g-1·h-1 with 100%selectivity,representing an order-of-magnitude enhancement compared with previous reports.The*O2-and*OH radicals formed from O2 and H2O oxidative cleave C-C and C-H bonds in polyethylene to CO2,which is subsequentially selective reduced to CO via multi-electron proton-coupling.This work offers a conceptual advance in designing dual-metal site catalysts,opening new avenues for cascading photocatalytic conversion of white pollution into valuable chemicals. 展开更多
关键词 Metal-organic framework Dual-metal sites Phase transformation Photocascade Plastic-to-fuel conversion
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Multivariate MOF-derived single-atom catalyst with enhanced site accessibility as a bifunctional electrocatalyst for zinc-air batteries 认领 引用
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作者 Guoxin Zhang Shaoqing Feng +5 位作者 Kairen Cheng Xingxing Li Jiangxia Tian Kai Chen Huile Jin Shun Wang 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第6期723-728,共6页
High-performance bifunctional oxygen electrocatalysts are urgently required for rechargeable zinc-air batteries(ZABs)due to sluggish kinetics of oxygen reduction/evolution reactions(ORR/OER)at the air cathode.In this ... High-performance bifunctional oxygen electrocatalysts are urgently required for rechargeable zinc-air batteries(ZABs)due to sluggish kinetics of oxygen reduction/evolution reactions(ORR/OER)at the air cathode.In this study,an iron single-atom catalyst(Fe-SAC,FeTCPP@UiO-66–800)is synthesized by direct pyrolysis of a metalloporphyrin-incorporated multivariate MOF.The spatial separation effect of the framework linkers endows Fe-SAC with hierarchical porosity,improved metal utilization efficiency,and enhanced site accessibility by suppressing the metal agglomeration during pyrolysis.Moreover,the possible formation of di-or tri-atomic iron sites facilitates the OER activity via the oxide pathway mechanism(OPM),contributing to the excellent bifunctional ORR/OER performance with aΔE of 0.59 V.Both liquid and flexible ZAB assembled with FeTCPP@UiO-66–800 demonstrate enhanced activity,long-term durability,and anti-deformation ability(340.5 mW/cm2peak power density in liquid device).This study presents a novel strategy for preparing MOF-derived SACs with highly accessible single-atom sites,offering a promising route to high-performance energy conversion devices. 展开更多
关键词 Multivariate MOF Iron single-atom catalyst Site accessibility Bifunctional electrocatalyst Zinc-air battery
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Superficial S atom optimized active sites in NiFe layered double hydroxides for electrocatalytic urea oxidation 认领 引用
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作者 Zhe Deng Xiandi Ma +5 位作者 Ning Wang Menggai Jiao Hao Wan Li-Li Zhang Wei Ma Zhen Zhou 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第5期189-199,共11页
Developing efficient electrocatalysts for the urea oxidation reaction(UOR)is a promising strategy for purifying urea-laden wastewater and promoting energy-efficient hydrogen production.However,the strong binding of th... Developing efficient electrocatalysts for the urea oxidation reaction(UOR)is a promising strategy for purifying urea-laden wastewater and promoting energy-efficient hydrogen production.However,the strong binding of the hydroxyl group to Fe sites in the NiFe layered double hydroxide(NiFe-LDH)impedes the generation of active Ni3+-O,thus raising the onset potential of UOR.Moreover,identifying and tracking the active sites in NiFe-LDH at the molecular level remains a considerable challenge during the UOR process.Herein,we modified NiFe-LDH by incorporating the low-electronegativity S element to create S-NiFe-LDH,thereby optimizing the electron structure and facilitating the transfer of active sites from Ni2+and Fe3+in the original NiFe-LDH to high-valence Ni intermediates in S-NiFe-LDH at a low applied potential.Moreover,the incorporation of S into NiFe-LDH significantly reduces the thermodynamic barrier of the Ni active sites,advancing the intrinsic activity and kinetic process of the active sites for the decomposition of urea by facilitating the Ni3+-O formation because of the facile dehydrogenation steps at the Ni sites.As a result,the S-NiFe-LDH achieved excellent electrochemical UOR activity,with a low potential of 1.36 V and long-term durability at 100 mA cm-2,demonstrating promising prospects for practical application.Overall,this work unscrambles the immediate active sites during electrocatalysis and paves a new avenue for the electronic engineering of NiFe-based catalysts in the UOR process. 展开更多
关键词 Urea oxidation reaction S doping NiFe layered hydroxide Surface reconstruction Active sites
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Interface effect induced electron-deficient Ni sites for efficient glycerol electrooxidation 认领 引用
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作者 Lan Tang Ji Chen +5 位作者 Yucheng Wu Linxin Qi Xingyi Tian Ming Li Wenbin Wang Rongxing He 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第6期646-651,共6页
Glycerol oxidation reaction has got lots of attention in an electrocatalytic system of simultaneous hydrogen production and valuable chemicals generation.However,the lack of electrochemical dehydrogenation capability ... Glycerol oxidation reaction has got lots of attention in an electrocatalytic system of simultaneous hydrogen production and valuable chemicals generation.However,the lack of electrochemical dehydrogenation capability of the active phase is hard to deliver a large current density at a low potential.Furthermore,high selectivity of products is also still far from being completed due to the adsorption-desorption disequilibrium of glycerol and the obtained products,reducing the economic feasibility and limiting the practical application.Here,we propose a strategy to boost the electrocatalytic glycerol oxidation through electron-deficient Ni sites induced by electron transfer of heterojunction interface.Taking Ni3S2/Cu2S as a pre-catalysts,we demonstrate that the electron-deficient Ni site can favor the dehydrogenation of the active phase to facilitate the rapid transformation of Ni2+/Ni3+in the electrooxidation process of glycerol.Furthermore,electron deficient Ni sites balance competitive adsorption of active species,improving the activity and selectivity of glycerol oxidation.As expected,the electrocatalysts exhibit selectivity of 93.3%for formate at the 1.35 V,and require only 1.45 V to drive an industrial-level current densities of 600 mA/cm2.This work provides valuable insights into constructing highly active and selective electrocatalysts for organic electrosynthesis in hybrid water electrolysis. 展开更多
关键词 Electron-deficient site Heterojunction interface Formate Glycerol electrooxidation High selectivity
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Isolated Pt sites anchored by skeletal Fe in MFI zeolite nanosheets towards productive propane dehydrogenation 认领 引用
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作者 Xintong Lv Zhengchang Wei +3 位作者 Xin Deng Yuchao Chai Guangjun Wu Landong Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第5期61-73,共13页
The development of effective alkane dehydrogenation catalysts is essential to produce olefins from abundant shale gas.Commercial Pt-based propane dehydrogenation catalysts suffer from deactivation due to sintering and... The development of effective alkane dehydrogenation catalysts is essential to produce olefins from abundant shale gas.Commercial Pt-based propane dehydrogenation catalysts suffer from deactivation due to sintering and coke deposition,highlighting the need for substantial improvements in thermal stability and production efficiency.Herein,we present a facile one-pot strategy to create atomically dispersed bimetallic Pt-O-Fe motifs encapsulated within MFI zeolite nanosheet,serving as highly active and stable sites for propane dehydrogenation.Comprehensive characterization results reveal that the skeletal Fe(III)species in MFI zeolite act as anchoring sites,thereby stabilizing atomically dispersed Pt species through the unique linkages of≡Si-O-Fe-O-Pt.The optimized 0.3Pt2Fe@NS catalyst,featuring high skeletal Fe content,low Pt loading,and ideal synergetic effect of Pt-Fe endowed by the suitable Pt-to-Fe ratio,achieves a propylene productivity of 48.0 mmol C3H6·gcat-1·h-1 with>95%selectivity at 550℃for 30 h without performance degradation.The 0.3Pt2Fe@NS catalyst also exhibits complete regenerability under harsh cycling conditions,establishing a new structure-performance paradigm for the design of industrial PDH catalysts. 展开更多
关键词 Propane dehydrogenation Isolated platinum Skeletal iron MFI zeolite nanosheets Bimetallic sites
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Engineering of Asymmetric Dual-Atom Sites for Effective Oxygen Electrocatalysis 认领 引用
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作者 Dongping Xue Yu Zhao +1 位作者 Jianliang Cao Yan Wang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2026年第9期516-562,共47页
Asymmetric dual-atom site catalysts(ADASCs)inherit the high atomic utilization of single-atom site catalysts and synergistic effects of symmetric dual-atom site catalysts,while uniquely integrating the asymmetry of he... Asymmetric dual-atom site catalysts(ADASCs)inherit the high atomic utilization of single-atom site catalysts and synergistic effects of symmetric dual-atom site catalysts,while uniquely integrating the asymmetry of heteronuclear metal centers and asymmetric coordination environments.This structural merit endows them with tunable electronic configurations and optimized reaction kinetics,breaking conventional catalysts'inherent limitations to boost catalytic performance significantly.Despite existing reviews on dual-atom site catalysts for electrocatalysis,a comprehensive asymmetry-focused framework to elucidate ADASCs'catalytic behaviors remains elusive.This review summarizes the multi-dimensional regulation mechanisms of ADASCs.Structurally,heteronuclear metal synergy and bridging ligand co-anchoring suppress single-atom agglomeration.Electronically,d-band center modulation,spin coupling,and orbital hybridization optimize intermediate adsorption energies.Subsequently,the strategies for constructing asymmetric structures are elaborated,including the design of heteronuclear metal centers and the regulation of asymmetric coordination environments via nonmetallic atom engineering.Furthermore,the prominent advantages of ADASCs in oxygen electrocatalysis are highlighted as their asymmetric configurations can break the linear scaling relationship of intermediate adsorption,and optimize the reaction pathway as well as the adsorption behaviors of key intermediates.Finally,the current challenges and opportunities of ADASCs are discussed,providing valuable insights for the development of high-performance energy conversion devices. 展开更多
关键词 Asymmetric dual-atom sites Synergetic effect Spin configuration Oxygen electrocatalysis
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Hybrid nanoparticle-single atom Pt sites strongly coupled on selfassembled Pd network for enhanced hydrogen evolution and oxygen reduction 认领 引用
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作者 Yongqing Shen Manyuan Gan +7 位作者 Zixuan Wang Yangrui Li Guodong An Bing Hao Xudong Wang Peizhi Liu Yanhui Song Junjie Guo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第6期49-59,I0003,共11页
The noble metal-based catalysts for hydrogen evolution reaction(HER)and oxygen reduction reaction(ORR)in alkaline electrolytes still confront fundamental challenges in balancing activity,durability,and metal utilizati... The noble metal-based catalysts for hydrogen evolution reaction(HER)and oxygen reduction reaction(ORR)in alkaline electrolytes still confront fundamental challenges in balancing activity,durability,and metal utilization efficiency,which severely impedes the industrial application of hydrogen energy.Herein,we design a hybrid catalyst by hosting dual-scale Pt sites(single atoms and nanoparticles)into a two-dimensional(2D)Pd network,enabling strong electronic coupling and efficient metal utilization.Owing to the self-assembled 2D Pd networks composed of coplanar Pd nanoparticles,which provide abundant anchoring sites for heteroatoms and nanochannels for mass transfer,and the coexistence of multiple active sites by controlling the ratio of Pt single atoms to nanoparticles,the optimized hybrid catalyst(Pt/Pd-5 nanomesh)exhibits exceptional HER activity(20 and 125 mV at 10 and 100 mA cm-2)and ORR activity(a mass activity of 1.66 A mg-PG1Mand a specific activity of 2.70 mA cm-2).In zinc-air batteries,Pt/Pd-5 nanomesh delivers an open-circuit voltage of 1.49 V and maintains stability for 300 h at10 m A cm-2.Combined experimental and computational studies confirm that the synergistic effects between the 2D Pd matrix and multiple Pt active sites not only optimize interfacial water dissociation in HER but also promote the conversion of*O→*OH species during ORR.Furthermore,the complementary characteristics of distinct active sites enable multifunctional cooperativity.This synergistic strategy between the matrix and metal sites may provide a guideline for developing efficient,robust,and multifunctional electrocatalysts. 展开更多
关键词 Multiple sites Synergistic catalytic effect Self-assembled nanomesh Hydrogen evolution reaction Oxygen reduction reaction
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Different natural iron-bearing minerals activated peroxymonosulfate for in-situ chemical oxidation process:Insights into the active Fe sites and activation mechanism 认领 引用
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作者 Jinyan Yang Ying Chen +5 位作者 Minghan Yu Lan Zhu Yilin Wang Jingsong Chen Hui Ma Shengyan Pu 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第7期343-351,共9页
In situ chemical oxidation(ISCO)technology using peroxymonosulfate(PMS)and natural iron-bearing minerals for groundwater remediation has received increasing interest.The interaction between PMS and active Fe sites in ... In situ chemical oxidation(ISCO)technology using peroxymonosulfate(PMS)and natural iron-bearing minerals for groundwater remediation has received increasing interest.The interaction between PMS and active Fe sites in minerals significantly influences the effectiveness of groundwater remediation.Nevertheless,there has been limited research investigating the relationship between the minerals active Fe sites and PMS activation.Herein,we distinguished and quantified the active Fe sites of common natural iron-bearing minerals in groundwater aquifers.Lewis acid sites(Fe-OH)were confirmed as the reaction sites in iron oxide/hydroxide/bearing clay minerals.The activation performance of minerals is positively correlated with their Lewis acid content.In iron sulfide minerals,Fe-S sites act as electron transfer mediators,facilitating PMS adsorption and activation.The activation of PMS by Lewis acid and Fe-S sites free radical both led to the generation of free radicals(SO4·-and·OH)for CPs removal.Moreover,typical ferrihydrite/PMS and pyrite/PMS systems exhibited resistance to environmental interference and broad pH adaptability.A one-dimensional sand column experiment further proved their feasibility and long-term applicability in saturated porous media.These findings highlight the critical influence of active Fe sites of natural iron-bearing minerals and provide technical support for the application of PMS-ISCO strategies for groundwater remediation. 展开更多
关键词 Groundwater remediation In situ chemical oxidation Natural iron-bearing minerals Peroxymonosulfate activation Active Fe sites
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Synergistic optimization of charge transfer and active sites in Bi12O17Br2/CuTCPP for efficient CO2 photoreduction 认领 引用
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作者 Tiange Wei Mengxia Ji +5 位作者 Yi Zhang Keke Wang Meng Wang Yuanbin She Jiexiang Xia Huaming Li 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第6期360-366,共7页
Utilizing sunlight to directly convert CO2into value-added chemicals presents a pivotal strategy for sustainable CO2conversion and mitigating environmental challenges.Herein,a surfacemounted 5,10,15,20-tetra(4-c... Utilizing sunlight to directly convert CO2into value-added chemicals presents a pivotal strategy for sustainable CO2conversion and mitigating environmental challenges.Herein,a surfacemounted 5,10,15,20-tetra(4-carboxyphenyl)porphyrin copper(Ⅱ)(CuTCPP)anchoringonBi12O17Br2nanotubes(CuTCPP/Bi12O17Br2)heterojunction was employed as an operable platformfor photocatalytic CO2reduction.The built-in electric field at the interface facilitates the efficient electron transfer from Bi12O17Br2to CuTCPP,significantly enhancing photoexcited charge separation and transfer kinetics.Besides,the Cu(Ⅱ)sites in CuTCPP act as supplementary catalytic centers that reduce the adsorption and activation energy barrier of CO2,thus accelerating the formation of *CO intermediates.The CuTCPP/Bi12O17Br2heterojunction exhibits enhanced photoreduction activity of CO2,achieving a CO evolution rate of 92.2μmol g-1h-1,which represents a 4.0-foldenhancement over Bi12O17Br2.This work offers new insights into the development of heterojunctions with synergistically optimized charge transfer and active sites. 展开更多
关键词 Charge transfer Active sites Cu porphyrin CO2photoreduction
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Unlocking high-rate MXenes as lithium-ion battery anodes viaΣ7 coincidence site lattice grain boundaries 认领 引用
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作者 Yifan Wu Zhongyong Zhang +3 位作者 Shangquan Zhao Bin Huang Neng Li Naigen Zhou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第5期31-37,I0003,共7页
Grain boundaries(GBs),particularlyΣ7 coincidence site lattice(CSL)defects experimentally observed in MXenes,significantly influence their performance as lithium-ion battery(LIB)anodes.This work systematically investi... Grain boundaries(GBs),particularlyΣ7 coincidence site lattice(CSL)defects experimentally observed in MXenes,significantly influence their performance as lithium-ion battery(LIB)anodes.This work systematically investigates the impact ofΣ7 GBs on MXene electrochemical properties,with a focus on rate capability.The results indicated thatΣ7 GB formation is thermodynamically favored in Ti2C,Nb2C,and Mo2C MXenes compared to other M2C compositions,with stability further enhanced by oxygen and sulfur surface functionalization.These GBs induce substantial geometric distortions that reduce surface charge localization while enhancing electrical conductivity in Ti2CO2.The altered electronic structure at GB sites weakens lithium adsorption strength without promoting lithium dendrite formation.Furthermore,diffusion kinetics calculations reveal significantly reduced lithium diffusion barriers atΣ7 GBs in Ti2C,Mo2C,and Mo2CS2compared to pristine materials.Mechanistic analysis attributes this enhancement to diminished charge localization at GB regions,which generates a“charge pool”effect—a zone of uniformly distributed free charge observed in Ti2C and Mo2C.This charge pool not only facilitates ultra-low lithium diffusion barriers(as low as 11 meV in M2C at 0.1 V vs.Li+/Li)but also enhances potential responsiveness of diffusion kinetics.Our findings establish the intentional introduction ofΣ7 GBs as an effective strategy for designing high-rate MXene anodes.This work provides fundamental insights into GB-enhanced electrochemical mechanisms in 2D materials,offering crucial theoretical guidance for the design of high-rate anode materials. 展开更多
关键词 MXenes Coincidence site lattice grain boundaries(CSL-GBs) High-rate anodes Charge pool effect Lithium-ion batteries
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Asymmetric oxygen-bridged Bi-In dual sites for efficient photothermal CO2 methanation 认领 引用
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作者 Mang Zheng Qi Li +4 位作者 Qianxi Liu Huiquan Gu Mingyang Liu Qi Liu Baojiang Jiang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第4期351-362,共12页
Photothermal coupling catalytic CO2/H2O to CH4 is recognized as an effective strategy for addressing environmental concerns and energy crisis.However,hydrogen evolution reaction(HER)competition and weak inter... Photothermal coupling catalytic CO2/H2O to CH4 is recognized as an effective strategy for addressing environmental concerns and energy crisis.However,hydrogen evolution reaction(HER)competition and weak intermediate adsorption limiting CH4 selectivity and yield during the reaction process.Herein,we incorporate Bi into the In2O3 lattice to create an oxygen-bridged asymmetric bimetallic In-O-Bi(In-O-Bi bridge)sites.The optimized Bi/In2O3 catalyst achieves CH4 yield of 214.1μmol·g-1 with 96.7%selectivity.The exceptional catalytic activity of Bi/In2O3 stems from two key synergistic effects:(1)the cooperative interaction between Bi and In as p-block metals effectively suppress the competing HER,and(2)the unique In-O-Bi bridge configuration induces significant electron delocalization through p-orbital hybridization.This electronic modulation creates highly active catalytic centers,with In sites preferentially facilitating H2O dissociation while Bi sites selectively promote CO2 reduction.Moreover,the electron delocalization effect in the In-O-Bi bridge sites enhances the adsorption and electron transfer capabilities of the Bi/In2O3 surface for key CHO species,and reduces the energy barrier,thereby enabling efficient CH4 production.These findings provide crucial insights into the design of photothermal catalysts,highlighting the transformative potential of oxygen-bridged asymmetric bimetallic units in efficient CO2 methanation and sustainable energy technologies. 展开更多
关键词 Photothermal catalysis CO2methanation Orbital hybridization Electron delocalization In-O-Bi bridge sites
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Microstructure regulation to manifold catalysis sites of magnetic hydrochar for enhancing Fenton-like degradation of tetracycline 认领 引用
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作者 Zijing Guo Yi Liang +5 位作者 Kaili He Hongru Jiang Xiang Liu Congying Xu Yawei Xiao Jihui Li 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第2期678-686,共9页
Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K2FeO4-involving hydrothermal oxidative magnetization w... Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K2FeO4-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar(MHC)for Fenton-like degradation of tetracycline in aqueous solution.Diverse shapes of Fe3O4 and nano zero-valent iron(nZVI)were doped with abundant oxygen containing groups and persistent free radicals(PFRs).Multiple catalysis sites including iron species,PFRs,oxygen containing groups,and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect.Notably,MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L,with a total organic carbon(TOC)removal rate of 35%.Furthermore,after four cycles of reuse,the degradation efficiency slightly decreased to 93%.This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants. 展开更多
关键词 Magnetic hydrochar Fenton-like degradation Diverse shapes of iron species Multiple catalysis sites Tetracycline
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Anogenital human papillomavirus infection patterns by anatomical site and sexual orientation in Chinese men:a national multi-center study 认领 引用
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作者 Shangying Hu Huan Yang +8 位作者 Jinyu Zhang Hongyang Yu Yutong Li Douhong Li Qiaoyun Du Yu Cui Xuelian Zhao Yongjiang Liu Fanghui Zhao 《Cancer Biology & Medicine》 SCIE CAS CSCD 2026年第7期1044-1050,共7页
Human papillomavirus(HPV)is the most prevalent sexually transmitted infection worldwide1.More than 200 HPV genotypes have been identified and are classified as high-risk HPV(HR-HPV)or low-risk HPV(LR-HPV)according to ... Human papillomavirus(HPV)is the most prevalent sexually transmitted infection worldwide1.More than 200 HPV genotypes have been identified and are classified as high-risk HPV(HR-HPV)or low-risk HPV(LR-HPV)according to their oncogenic potential.Persistent infection with HR-HPV is associated with cancers of the cervix,vagina,vulva,anus,penis,and oropharynx.In contrast,LR-HPV infections cause benign lesions,such as genital warts and recurrent respiratory papillomatosis. 展开更多
关键词 genital warts anatomical site sexual orientation sexually transmitted infection human papillomavirus infection benign lesionssuch human papillomavirus hpv recurrent respiratory papillomatosis
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