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Progress in MOF-based catalyst design and reaction mechanisms for CO_(2)hydrogenation to methanol
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作者 YU Zhifu JIANG Lei WU Mingbo 《燃料化学学报(中英文)》 北大核心 2026年第1期146-162,共17页
Against the backdrop of escalating global climate change and energy crises,the resource utilization of carbon dioxide(CO_(2)),a major greenhouse gas,has become a crucial pathway for achieving carbon peaking and carbon... Against the backdrop of escalating global climate change and energy crises,the resource utilization of carbon dioxide(CO_(2)),a major greenhouse gas,has become a crucial pathway for achieving carbon peaking and carbon neutrality goals.The hydrogenation of CO_(2)to methanol not only enables carbon sequestration and recycling,but also provides a route to produce high value-added fuels and basic chemical feedstocks,holding significant environmental and economic potential.However,this conversion process is thermodynamically and kinetically limited,and traditional catalyst systems(e.g.,Cu/ZnO/Al_(2)O_(3))exhibit inadequate activity,selectivity,and stability under mild conditions.Therefore,the development of novel high-performance catalysts with precisely tunable structures and functionalities is imperative.Metal-organic frameworks(MOFs),as crystalline porous materials with high surface area,tunable pore structures,and diverse metal-ligand compositions,have the great potential in CO_(2)hydrogenation catalysis.Their structural design flexibility allows for the construction of well-dispersed active sites,tailored electronic environments,and enhanced metal-support interactions.This review systematically summarizes the recent advances in MOF-based and MOF-derived catalysts for CO_(2)hydrogenation to methanol,focusing on four design strategies:(1)spatial confinement and in situ construction,(2)defect engineering and ion-exchange,(3)bimetallic synergy and hybrid structure design,and(4)MOF-derived nanomaterial synthesis.These approaches significantly improve CO_(2)conversion and methanol selectivity by optimizing metal dispersion,interfacial structures,and reaction pathways.The reaction mechanism is further explored by focusing on the three main reaction pathways:the formate pathway(HCOO*),the RWGS(Reverse Water Gas Shift reaction)+CO*hydrogenation pathway,and the trans-COOH pathway.In situ spectroscopic studies and density functional theory(DFT)calculations elucidate the formation and transformation of key intermediates,as well as the roles of active sites,metal-support interfaces,oxygen vacancies,and promoters.Additionally,representative catalytic performance data for MOFbased systems are compiled and compared,demonstrating their advantages over traditional catalysts in terms of CO_(2)conversion,methanol selectivity,and space-time yield.Future perspectives for MOF-based CO_(2)hydrogenation catalysts will prioritize two main directions:structural design and mechanistic understanding.The precise construction of active sites through multi-metallic synergy,defect engineering,and interfacial electronic modulation should be made to enhance catalyst selectivity and stability.In addition,advanced in situ characterization techniques combined with theoretical modeling are essential to unravel the detailed reaction mechanisms and intermediate behaviors,thereby guiding rational catalyst design.Moreover,to enable industrial application,challenges related to thermal/hydrothermal stability,catalyst recyclability,and cost-effective large-scale synthesis must be addressed.The development of green,scalable preparation methods and the integration of MOF catalysts into practical reaction systems(e.g.,flow reactors)will be crucial for bridging the gap between laboratory research and commercial deployment.Ultimately,multi-scale structure-performance optimization and catalytic system integration will be vital for accelerating the industrialization of MOF-based CO_(2)-to-methanol technologies. 展开更多
关键词 CO_(2)hydrogenation metal-organic frameworks(MOFs) catalyst design reaction mechanism METHANOL
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Recent advancement and future challenges of photothermal catalysis for VOCs elimination:From catalyst design to applications 被引量:9
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作者 Yang Yang Shenghao Zhao +7 位作者 Lifeng Cui Fukun Bi Yining Zhang Ning Liu Yuxin Wang Fudong Liu Chi He Xiaodong Zhang 《Green Energy & Environment》 SCIE EI CAS CSCD 2023年第3期654-672,共19页
Photothermal catalysis realizes the synergistic effect of solar energy and thermochemistry,which also has the potential to improve the reaction rate and optimize the selectivity.In this review,the research progress of... Photothermal catalysis realizes the synergistic effect of solar energy and thermochemistry,which also has the potential to improve the reaction rate and optimize the selectivity.In this review,the research progress of photothermal catalytic removal of volatile organic compounds(VOCs)by nano-catalysts in recent years is systematically reviewed.First,the fundamentals of photothermal catalysis and the fabrication of catalysts are described,and the design strategy of optimizing photothermal catalysis performance is proposed.Second,the performance for VOC degradation with photothermal catalysis is evaluated and compared for the batch and continuous systems.Particularly,the catalytic mechanism of VOC oxidation is systematically introduced based on experimental and theoretical study.Finally,the future limitations and challenges have been discussed,and potential research directions and priorities are highlighted.A broad view of recent photothermal catalyst fabrication,applications,challenges,and prospects can be systemically provided by this review. 展开更多
关键词 Photothermal catalysis VOCS catalyst design Light-driven thermal catalysis Photothermal synergistic effect
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STRUCTURE OF CATALYST DESIGN KNOWLEDGE BASE SYSTEM
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作者 滕至阳 程正潮 +1 位作者 姜浩 沈军 《Journal of Southeast University(English Edition)》 EI CAS 1992年第1期84-91,共8页
A knowledge base system INCAP(Integration of Catalyst Activity Patterns)for selecting catalyst components has been developed by decomposing the catalyst designproblem into 5 easily solved sub-problems and by building ... A knowledge base system INCAP(Integration of Catalyst Activity Patterns)for selecting catalyst components has been developed by decomposing the catalyst designproblem into 5 easily solved sub-problems and by building up a weighted experimental es-timation model of catalytic activity for application of activity data.The INCAP was ap-plied to the design of catalysts for oxidative dehydrogenation of ethylbeneze and the re-sults are in agreement with the experimental ones.The characters of INCAP are analyzedfrom the view of design expert system. 展开更多
关键词 COMPUTER CHEMISTRY catalyst design EXPERT SYSTEM
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From LLM to Agent:A large-language-model-driven machine learning framework for catalyst design of MgH_(2)dehydrogenation
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作者 Tongao Yao Yang Yang +7 位作者 Jianghao Cai Rui Liu Zhaoyan Dong Xiaotian Tang Xuqiang Shao Zhengyang Gao Guangyao An Weijie Yang 《Journal of Magnesium and Alloys》 2026年第1期410-426,共17页
Magnesium hydride(MgH_(2)),a promising high-capacity hydrogen storage material,is hindered by slow dehydrogenation kinetics.AIdriven catalyst discovery to address this is often hampered by the laborious extraction of ... Magnesium hydride(MgH_(2)),a promising high-capacity hydrogen storage material,is hindered by slow dehydrogenation kinetics.AIdriven catalyst discovery to address this is often hampered by the laborious extraction of data from unstructured literature.To overcome this,we introduce a transformative“LLM to Agent”framework that synergistically integrates Large Language Models(LLMs)for automated data curation with Machine Learning(ML)for predictive design.We automatically constructed a comprehensive database of 809 MgH_(2)catalysts(6555 data rows)with high fidelity and an~40-fold acceleration over manual methods.The resulting ML models achieved high accuracy(average R^(2)>0.91)in predicting dehydrogenation temperature and activation energy,subsequently guiding a Genetic Algorithm(GA)in an exploratory inverse design that autonomously uncovered key design principles for high-performance catalysts.Encouragingly,a strong alignment was found between these AI-discovered principles and the design strategies of recently reported,state-of-the-art experimental systems,providing substantial evidence for the validity of our approach.The framework culminates in Cat-Advisor,a novel,domain-adapted multi-agent system.Cat-Advisor translates ML predictions and retrieval-augmented knowledge into actionable design guidance,demonstrating capabilities that surpass those of general-purpose LLMs in this specialized domain.This work delivers a practical AI toolkit for accelerated materials discovery and advances the emerging Agent-based paradigm for designing next-generation energy technologies. 展开更多
关键词 MgH_(2)dehydrogenation Large language model Machine learning Genetic algorithm catalyst design Hydrogen storage
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Iridium-based electrocatalysts for oxygen evolution reaction in acidic media:From in situ characterization to rational design
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作者 Bo Sun Haoyan Cheng +5 位作者 Kexing Song Zhonghan Jiang Changrui Shi Hao Liang Shuaiyu Ma Hao Hu 《Journal of Energy Chemistry》 2025年第8期472-494,共23页
Proton exchange membrane water electrolyzer(PEMWE)is crucial for the storage and conversion of renewable energy.However,the harsh anode environment and the oxygen evolution reaction(OER),which involves a four-electron... Proton exchange membrane water electrolyzer(PEMWE)is crucial for the storage and conversion of renewable energy.However,the harsh anode environment and the oxygen evolution reaction(OER),which involves a four-electron transfer,result in a significant overpotential that limits the overall efficiency of hydrogen production.Identifying active sites in the OER is crucial for understanding the reaction mechanism and guiding the development of novel electrocatalysts with high activity,cost-effectiveness,and durability.Herein,we summarize the widely accepted OER mechanism in acidic media,in situ characterization and monitoring of active sites during the reaction,and provide a general understanding of the active sites on various catalysts in the OER,including Ir-based metals,Ir-based oxides,carbon/oxide-supported Ir,Ir-based perovskite oxides,and Ir-based pyrochlore oxides.For each type of electrocatalysts,reaction pathways and actual active sites are proposed based on in situ characterization techniques and theoretical calculations.Finally,the challenges and strategic research directions associated with the design of highly efficient Ir-based electrocatalysts are discussed,offering new insights for the further scientific advancement and practical application of acidic OER. 展开更多
关键词 Ir-based electrocatalysts Water splitting Acidic oxygen evolution In situ characterization Reaction mechanisms catalyst design
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Rational design of copper alloy electrocatalysts for electrocatalytic CO_(2) reduction
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作者 Lei Xue Yuntao Qi +3 位作者 Zhuo Li Huimin Yang Ruilin Liu Bin Zhang 《Journal of Energy Chemistry》 2025年第11期88-108,I0004,共22页
Electrocatalytic carbon dioxide reduction(CO_(2)RR)represents an innovative technology for energy conversion by converting CO_(2)into value-added multi-carbon fuels and chemicals,with copper(Cu)-based catalysts playin... Electrocatalytic carbon dioxide reduction(CO_(2)RR)represents an innovative technology for energy conversion by converting CO_(2)into value-added multi-carbon fuels and chemicals,with copper(Cu)-based catalysts playing a pivotal role as the only known metallic capable of driving such multi-carbon product formation.However,pure Cu catalysts suffer from intrinsic limitations,including suboptimal selectivity toward desired hydrocarbons due to unstable key intermediate,and rapid deactivation caused by catalyst surface reconstruction under operational conditions.Cu-based alloy catalysts address the challenges of low selectivity,poor stability,and high overpotential in the electrocatalytic reduction of CO_(2)by optimizing intermediate adsorption and enhancing reaction kinetics.This review systematically examines the catalytic mechanisms,design principles,and performance of Cu alloys in steering CO_(2)RR pathways toward key products(CO,HCOOH,CH_(4),C_(2)H_(4),and C_(2+)alcohols).By alloying Cu with secondary metals(e.g.,Ag,Zn,Sn,or rare-earth elements),bimetallic electronic effects modulate intermediate adsorption energetics(^(*)CO,^(*)COOH,^(*)OCHO)and enhance C–C coupling kinetics.We propose future directions integrating in situ characterization and machine learning-driven alloy design to bridge fundamental understanding with industrial application.This work provides a comprehensive roadmap for developing nextgeneration Cu alloy catalysts to enable efficient CO_(2)valorization in a carbon–neutral energy landscape. 展开更多
关键词 Cu alloy Reaction mechanism catalyst design strategy DFT CO_(2)reduction reactions
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Catalyst design for ammonia decomposition:an overview
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作者 Tong Han Lu Wei +3 位作者 Shaohua Xie Yuxi Liu Hongxing Dai Jiguang Deng 《Industrial Chemistry & Materials》 2025年第3期311-331,共21页
Ammonia serves as a viable medium for hydrogen storage owing to its significant hydrogen content and elevated energy density,and the absence of carbon dioxide emissions during ammonia-to-hydrogen production has inspir... Ammonia serves as a viable medium for hydrogen storage owing to its significant hydrogen content and elevated energy density,and the absence of carbon dioxide emissions during ammonia-to-hydrogen production has inspired more research on ammonia decomposition.Despite growing interest,a significant gap persists between the depth of existing studies and the practical approach to on-the-spot hydrogen generation using ammonia decomposition.The creation of effective and accessible catalysts to feed ammonia decomposition is a critical step in addressing this daunting challenge.This paper systematically summarizes four key catalyst design strategies,including size effect,alkalinity modulation,metal-support interactions,and alloying,informed by experimental and theoretical investigations into ammonia decomposition.Each strategy's underlying mechanism for enhancing ammonia decomposition is elucidated in detail.Moreover,the paper categorizes catalysts employed in existing ammonia decomposition reactors to guide future catalyst development.The influence of diverse energy sources and reactor configurations on catalyst performance is also discussed to provide a comprehensive framework for advancing ammonia decomposition catalyst research. 展开更多
关键词 Ammonia decomposition reaction catalyst design Particle size effect Adjustment of alkalinity Strong metal–support interaction Alloying effect.
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Electrospun nanofibers for electrochemical reduction of CO_(2): From spinning fabrication techniques to electrocatalyst design
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作者 Yanbiao Liu Ping Feng +4 位作者 Zhenzhen Wang Yan Yan Yong Zheng Yu Zhang Mingkai Liu 《Nano Research》 2025年第2期80-100,共21页
Electrochemical reduction of CO_(2)(ECO_(2)RR)into value-added fuels and chemicals presents a promising avenue for mitigating CO_(2) emissions while simultaneously contributing to economic growth,thereby addressing cr... Electrochemical reduction of CO_(2)(ECO_(2)RR)into value-added fuels and chemicals presents a promising avenue for mitigating CO_(2) emissions while simultaneously contributing to economic growth,thereby addressing critical environmental and energy challenges.However,the large-scale implementation of ECO_(2)RR is significantly impeded by the necessity to design efficient catalysts that exhibit both high activity and selectivity.These catalysts must overcome the sluggish kinetics associated with ECO_(2)RR as well as the competing hydrogen evolution reaction.In recent decades,electrospun nanofibers have garnered considerable attention as potential catalysts for ECO_(2)RR,attributable to their high surface area with abundant active sites,tunable functionalities,and enhanced selectivity.This review comprehensively examines the rational design of ECO_(2)RR catalysts utilizing electrospinning technology.We commence with an in-depth exploration of the principles underlying the electrospinning process and subsequently summarize key factors influencing this process,including solution parameters,environmental conditions,and electrospinning operational parameters.Moreover,we discuss recent advancements in ECO_(2)RR catalysts synthesized through electrospinning,encompassing carbon nanofibers,composite nanofibers,and metal nanofibers.Finally,we delineate future perspectives and the challenges that electrospun materials face in the context of ECO_(2)RR applications.This review aims to inspire high-quality research directed toward the advancement of electrospun materials for improved performance in ECO_(2)RR. 展开更多
关键词 CO_(2)reduction reaction catalyst design ELECTROSPINNING single-atom catalysts
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Designing Oxide Catalysts for Oxygen Electrocatalysis: Insights from Mechanism to Application 被引量:6
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作者 Ning Han Wei Zhang +7 位作者 Wei Guo Hui Pan Bo Jiang Lingbao Xing Hao Tian Guoxiu Wang Xuan Zhang Jan Fransaer 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第10期514-546,共33页
The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both hav... The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges. 展开更多
关键词 Oxygen evolution Oxygen reduction Oxide catalysts catalyst design Fuel cell Metal–air batteries
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Electrosynthesis of H_(2)O_(2) through a two-electron oxygen reduction reaction by carbon based catalysts:From mechanism,catalyst design to electrode fabrication 被引量:4
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作者 Jingkun An Yujie Feng +3 位作者 Qian Zhao Xin Wang Jia Liu Nan Li 《Environmental Science and Ecotechnology》 SCIE 2022年第3期1-31,共31页
Hydrogen peroxide(H_(2)O_(2))is an efficient oxidant with multiple uses ranging from chemical synthesis to wastewater treatment.The in-situ H_(2)O_(2)production via a two-electron oxygen reduction reaction(ORR)will br... Hydrogen peroxide(H_(2)O_(2))is an efficient oxidant with multiple uses ranging from chemical synthesis to wastewater treatment.The in-situ H_(2)O_(2)production via a two-electron oxygen reduction reaction(ORR)will bring H_(2)O_(2)beyond its current applications.The development of carbon materials offers the hope for obtaining inexpensive and high-performance alternatives to substitute noble-metal catalysts in order to provide a full and comprehensive picture of the current state of the art treatments and inspire new research in this area.Herein,the most up-to-date findings in theoretical predictions,synthetic methodologies,and experimental investigations of carbon-based catalysts are systematically summarized.Various electrode fabrication and modification methods were also introduced and compared,along with our original research on the air-breathing cathode and three-phase interface theory inside a porous electrode.In addition,our current understanding of the challenges,future directions,and suggestions on the carbon-based catalyst designs and electrode fabrication are highlighted. 展开更多
关键词 H_(2)O_(2)production Oxygen reduction reaction Catalytic mechanism catalyst design Electrode fabrication
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Design strategies and structure‐performance relationships of heterogeneous catalysts for selective hydrogenation of 1,3‐butadiene 被引量:2
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作者 Mengru Wang Yi Wang +2 位作者 Xiaoling Mou Ronghe Lin Yunjie Ding 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第4期1017-1041,共25页
Selective hydrogenation of 1,3‐butadiene is an essential process in the upgrading of the crude C4 cut from the petroleum chemical sector.Catalyst design is crucial to achieve a virtually alkadiene‐free product while... Selective hydrogenation of 1,3‐butadiene is an essential process in the upgrading of the crude C4 cut from the petroleum chemical sector.Catalyst design is crucial to achieve a virtually alkadiene‐free product while avoiding over‐hydrogenating valuable olefins.In addition to the great industrial relevance,this demanding selectivity pattern renders 1,3‐butadiene hydrogenation a widely used model reaction to discriminate selective hydrogenation catalysts in academia.Nonetheless,critical reviews on the catalyst development are extremely lacking in literature.In this review,we aim to provide the reader an in‐depth overview of different catalyst families,particularly the precious metal‐based monometallic catalysts(Pd,Pt,and Au),developed in the last half century.The emphasis is placed on the development of new strategies to design high‐performance architectures,the establishment of structure‐performance relationships,and the reaction and deactivation mechanisms.Thrilling directions for future optimization of catalyst formulations and engineering aspect are also provided. 展开更多
关键词 1 3‐Butadiene catalyst design Selective hydrogenation Structure‐performance relationship Reaction and deactivation mechanism
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Direct synthesis of jet fuel range alkanes with lignocellulosic ketones and/or alcohols over a single non-noble metal catalyst
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作者 Zhufan Zou Aiqin Wang +2 位作者 Tao Zhang Yu Cong Ning Li 《Journal of Energy Chemistry》 2025年第9期101-108,I0005,共9页
C-C coupling and hydrodeoxygenation are two important reactions in the production of sustainable aviation fuels(SAFs)with lignocellulose derived oxygenates.However,it is challenging to integrate them into a one-step p... C-C coupling and hydrodeoxygenation are two important reactions in the production of sustainable aviation fuels(SAFs)with lignocellulose derived oxygenates.However,it is challenging to integrate them into a one-step process because the necessity of oxygen containing functional groups in the C-C coupling reactions.Herein,jet fuel range polycycloalkanes and branched alkanes were directly synthesized by a cascade self-aldol condensation/hydrodeoxygenation reaction of lignocellulosic ketones over a zirconium phosphate loaded calcium modified nickel catalyst(NiCa/ZrP)that was prepared by a simple incipient impregnation method.Compared with the catalyst systems that have been reported in literature,the NiCa/ZrP catalyst have many advantages such as fewer step,easier operation and preparation,lower equipment investment and cost,wider applicability,etc.Moreover,the NiCa/ZrP is also applicable for the direct production of jet fuel range alkanes with lignocellulosic ketones and/or alcohols by a cascade dehydrogenation/aldol condensation/hydrodeoxygenation reaction.This work gives a new idea about the reduction of energy consumption and cost by catalyst designing in the manufacture of SAFs from lignocellulose. 展开更多
关键词 LIGNOCELLULOSE KETONE Jet fuel Process integration catalyst design
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Advances in Multiple Active Site Catalysts for Urea Synthesis via Electrocatalytic C–N Coupling
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作者 Yihang Yu Jingwei Li +7 位作者 Zhongwei Yue Meiting Guo Zhishan Li Mohamed Nawfal Ghazzal Wei Li San Ping Jiang Yi-Bing Cheng Jianyun Zheng 《Transactions of Tianjin University》 2025年第5期478-497,共20页
Electrocatalytic C–N coupling technology offers a promising route for green and sustainable urea synthesis.However,this route faces challenges of low urea yield and Faradaic efficiency due to the high dissociation en... Electrocatalytic C–N coupling technology offers a promising route for green and sustainable urea synthesis.However,this route faces challenges of low urea yield and Faradaic efficiency due to the high dissociation energy of atomic bonds in reactants,complex reaction intermediates,high reaction energy barriers,and competing side reactions.As C–N coupling involves the synergistic action of two or more active sites,it is crucial to develop efficient multi-active-site catalysts to address these challenges.This review analyzes the reaction mechanisms of electrocatalytic C–N coupling for urea synthesis and summarizes effective strategies to achieve multi-active-site catalysts,including heteroatom doping,defect engineering,heterojunctions,and diatomic catalysts.Furthermore,based on this analysis,we propose the universal design principles for high-efficiency multi-activesite catalysts. 展开更多
关键词 ELECTROCATALYSIS UREA catalyst design C-N coupling Multi-active-site catalyst
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Perspective about gasoline soot combustion over ceria catalysts:A close look into the"active oxygen"enigma
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作者 Zilin Tu Gongde Wu +3 位作者 Changlong Zheng Xiaodong Wu Jie Wan Shuang Liu 《Journal of Rare Earths》 2025年第4期641-659,I0001,共20页
Catalyzed gasoline particulate filters(cGPFs)are being developed to enable compliance with the particulate number limits for passenger cars equipped with gasoline direct injection(GDI)engines in China and Europe,It is... Catalyzed gasoline particulate filters(cGPFs)are being developed to enable compliance with the particulate number limits for passenger cars equipped with gasoline direct injection(GDI)engines in China and Europe,It is appealing to build catalysts with ceria—an irreplaceable"reducible"component in three-way converters—to help eliminate the soot particles trapped in cGPFs via O_(2)-assisted combustion.While research aiming at understanding how these recipes function has continued for more than two decades,a universal model elucidating the roles of different"active oxygen"species is yet to be realized.In this perspective,by critically assessing the reported data about gasoline soot catalytic combustion over ceria catalysts,it is suggested that ceria ignites soot through contributing its lattice oxygen,giving rise to a"hot ring"region at the periphery of soot-catalyst interface.During the"re-oxidation"semi-cycles,electrophilic superoxides and/or peroxides(O_(x)^(n-))are produced at the Ce^(3+)and oxygen vacancy sites enriched in this collar-like region,and then work as key reactive phases for soot deep oxidation.Based on this"O_(x)^(n-)assisted"Mars-van Krevelen mechanism,several guidelines for ceria catalyst designing are proposed,ending with a summary about where future opportunities and challenges may lie in developing efficient and practical cGPF catalysts. 展开更多
关键词 Gasoline particulate filter Soot combustion Ceria catalysts Rare earths Reaction mechanism catalyst design
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Highly regioselective hydrogermylation of unsaturated C-C bonds over ligand-control single atom palladium catalysts
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作者 Junyou Ding Xiaotong Li +5 位作者 Hongmin Lin Bochao Ye Xing Zhou Feihu Cui Yingming Pan Haitao Tang 《Chinese Chemical Letters》 2025年第11期345-351,共7页
The selective addition reaction of unsaturated C-C bonds has always been a classic and constant research topic.Different from well-developed hydroboration,hydrosilylation,and hydrostannylation reaction,hydrogermylatio... The selective addition reaction of unsaturated C-C bonds has always been a classic and constant research topic.Different from well-developed hydroboration,hydrosilylation,and hydrostannylation reaction,hydrogermylation reaction remains challenging which hasn't been much reported.Herein,we developed a new metal-porous ligand polymers Pd1@POL-PPh_(n)Cy_(m)(n+m=3)with monoatomic dispersion characteristics for highly selective and efficient hydrogermylation of unsaturated C-C bonds,including alkynes,alkenes,and allenes.X-ray photoelectron spectroscopy and theoretical calculations further proved the introduction of cyclohexyl could gently adjust the charge on monoatomic Pd center which effectively facilitate the recognition and transformation of various substrates.With the electrically fine-tuned single atom palladium catalysts,we realized theα-germanium addition for the first time,obtaining corresponding allyl germanium and alkyl germanium compounds. 展开更多
关键词 Hydrogermylation Unsaturated C-C bonds Single atom catalyst catalyst design Regio-and stereo-selectivity
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Design strategies for enhancing the synthesis of C_(3+)products from electrochemical CO_(2) reduction
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作者 Yan Huang De-Sheng Zheng +1 位作者 Wen-Chuan Lai Zhi-Yuan Gu 《Journal of Energy Chemistry》 2025年第11期197-218,I0007,共23页
The electrochemical CO_(2)reduction reaction(eCO_(2)RR)offers significant potential for closing the anthropogenic carbon cycle while simultaneously enabling the storage of intermittent sustainable energy.The synthesis... The electrochemical CO_(2)reduction reaction(eCO_(2)RR)offers significant potential for closing the anthropogenic carbon cycle while simultaneously enabling the storage of intermittent sustainable energy.The synthesis of C_(3+)products from eCO_(2)RR is particularly appealing due to their higher commercial value compared to C_(1) or C_(2) compounds,and their crucial roles as high-energy-density fuels or feedstocks for a wide range of industrial applications.This encourages us to summarize recent notable progress in enhancing C_(3+)production.This review starts from the formation pathways of C_(3+)products by delving into key intermediates and ^(*)C–^(*)C coupling reactions for mechanistic investigations.Subsequently,we discuss the representative eCO_(2)RR electrocatalysts for C_(3+)synthesis,including Cu and non-Cu catalysts,highlighting typical design strategies for markedly promoting the catalytic performance or expanding the range of products.Additionally,we also emphasize system upgrading strategies,covering manipulation of electrolysis conditions,microenvironment regulation,and cascade catalysis,for facilitating C_(3+)production.We finally end with future directions in this rapidly advancing field.By elucidating the formation mechanisms,catalyst design principles,and system upgrading strategies,this review is expected to draw significant attention to C_(3+)products and stimulate further research into developing advanced catalytic systems for their efficient synthesis. 展开更多
关键词 Electrochemical CO_(2)reduction reaction(eCO_(2)RR) C_(3+)products Reaction mechanism catalyst design System upgrading
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Design and operando/in situ characterization of precious-metal-free electrocatalysts for alkaline water splitting 被引量:12
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作者 Tingwen Zhao Yuan Wang +3 位作者 Siva Karuturi Kylie Catchpole Qiang Zhang Chuan Zhao 《Carbon Energy》 CAS 2020年第4期582-613,共32页
Electrochemical water splitting has attracted considerable attention for the production of hydrogen fuel by using renewable energy resources.However,the sluggish reaction kinetics make it essential to explore precious... Electrochemical water splitting has attracted considerable attention for the production of hydrogen fuel by using renewable energy resources.However,the sluggish reaction kinetics make it essential to explore precious-metal-free electrocatalysts with superior activity and long-term stability.Tremendous efforts have been made in exploring electrocatalysts to reduce the energy barriers and improve catalytic efficiency.This review summarizes different categories of precious-metal-free electrocatalysts developed in the past 5 years for alkaline water splitting.The design strategies for optimizing the electronic and geometric structures of electrocatalysts with enhanced catalytic performance are discussed,including composition modulation,defect engineering,and structural engineering.Particularly,the advancement of operando/in situ characterization techniques toward the understanding of structural evolution,reaction intermediates,and active sites during the water splitting process are summarized.Finally,current challenges and future perspectives toward achieving efficient catalyst systems for industrial applications are proposed.This review will provide insights and strategies to the design of precious-metalfree electrocatalysts and inspire future research in alkaline water splitting. 展开更多
关键词 alkaline water splitting catalysts design ELECTROcatalystS operando/in situ characterization precious-metal-free catalysts
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Modeling and optimization of methane dry reforming over Ni-Cu/Al_2O_3 catalyst using Box-Behnken design 被引量:5
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作者 Seyedeh Molood Masoom Nataj Seyed Mehdi Alavi Golshan Mazloom 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2018年第5期1475-1488,共14页
In this work the effects of the contents of nickel (5, 7.5, 10 wt%) and copper (0, 1, 2 wt%) and reac- tion temperature (650, 700, 750 ℃) on the catalytic performance of Ni-Cu/Al_2O_3 catalyst in methane dry re... In this work the effects of the contents of nickel (5, 7.5, 10 wt%) and copper (0, 1, 2 wt%) and reac- tion temperature (650, 700, 750 ℃) on the catalytic performance of Ni-Cu/Al_2O_3 catalyst in methane dry reforming were evaluated using Box-Behnken design in order to optimize methane conversion, H_2/CO ratio and the catalyst deactivation. Different catalysts were prepared by co-impregnation method and characterized by XRD, BET, H_2-TPR, FESEM and TG/DTA analyses. The results revealed that copper addi- tion improved the catalyst reducibility. Promoted catalyst with low amounts of Cu gave higher activity and stability with high resistance to coke deposition and agglomeration of active phase especially during the reaction. However catalysts with high amounts of Cu were less active and rather deactivated due to the active sites sintering as well as Ni covering by Cu-enriched phase. The optimal conditions were de- termined by desirability function approach as 10 wt% of Ni, 0.83 wt% of Cu at 750℃. CH_4 conversion of 95.1%, H_2/CO ratio of 1 and deactivation of 1.4% were obtained experimentally under optimum conditions, which were in close agreement with the values oredicted hv the developed model. 展开更多
关键词 Methane dry reforming Copper addition Ni-based catalyst SYNGAS Box-Behnken design
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Renewal Design of Marketplace Culture Spaces in Traditional Blocks Based on Catalyst Theory: A Case Study of Pengzhen Town in Shuangliu District of Chengdu 被引量:1
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作者 NIE Kangcai ZHOU Xuehong 《Journal of Landscape Research》 2019年第4期10-13,18,共5页
In this study, three kinds of spaces with different marketplace atmospheres, namely, the tea-drinking space, the commercial space and the courtyard space, are created with the aid of the marketplace culture characteri... In this study, three kinds of spaces with different marketplace atmospheres, namely, the tea-drinking space, the commercial space and the courtyard space, are created with the aid of the marketplace culture characteristics of the local blocks in Pengzhen Town and the catalyst theory, so as to achieve the purpose of activating the traditional blocks in Pengzhen Town. The design takes the marketplace culture as the entry point and the most vigorous points as the catalyst points to create a living space with strong marketplace flavor, thereby activating the economic and social activities of the traditional block and promotes the sustainable renewal of the cultural space. 展开更多
关键词 catalyst THEORY Traditional DISTRICT MARKETPLACE CULTURE RENEWAL design
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基于机器学习筛选甘油氧化Pt/MO_(x)催化剂设计的综合实验
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作者 闫昊 李亚倩 +3 位作者 冯翔 刘熠斌 陈小博 杨朝合 《实验室研究与探索》 北大核心 2026年第1期143-147,173,共6页
在化工研究智能化转型的背景下,本研究聚焦于“甘油氧化Pt/MO_(x)催化剂设计”,依托机器学习在催化剂高通量筛选与跨尺度建模方面的进展,融合人工智能与机理建模方法,通过数据增强、特征工程与主动学习策略,实现了界面均一型催化剂的定... 在化工研究智能化转型的背景下,本研究聚焦于“甘油氧化Pt/MO_(x)催化剂设计”,依托机器学习在催化剂高通量筛选与跨尺度建模方面的进展,融合人工智能与机理建模方法,通过数据增强、特征工程与主动学习策略,实现了界面均一型催化剂的定向优化。实验设计紧跟学科前沿,结合计算机技术和化工专业知识,实验内容涉及软件操作、数据分析等内容,注重在实践的过程中培养学生的创新思维、实践操作能力和批判性思维,有助于促进教学质量的提升。 展开更多
关键词 甘油酸 机器学习 催化剂设计 实验设计
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