The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most s...The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most significant applications of metal oxides is heterogeneous catalysis,which represents a pivotal technology in industrial production on a global scale.Catalysts serve as the primary enabling agents for chemical reactions,and among the plethora of catalysts,metal oxides including magnesium oxide(MgO),ceria(CeO_(2))and titania(TiO_(2)),have been identified to be particularly effective in catalyzing a variety of reactions[1].Theoretical calculations based on density functional theory(DFT)and a multitude of other quantum chemistry methods have proven invaluable in elucidating the mechanisms of metal-oxide-catalyzed reactions,thereby facilitating the design of high-performance catalysts[2].展开更多
Single-atom catalysis has revolutionized heterogeneous catalysis,which offers unparalleled atomic efficiency,well-defined active sites,and unique electronic properties.Unlike traditional nanoparticle catalysts,single-...Single-atom catalysis has revolutionized heterogeneous catalysis,which offers unparalleled atomic efficiency,well-defined active sites,and unique electronic properties.Unlike traditional nanoparticle catalysts,single-atom catalysts(SACs)maximize metal utilization and exhibit distinct catalytic behaviors due to their atomically dispersed nature.Over the past decade,SACs have demonstrated exceptional performance in various electrochemical and thermocatalytic reactions[1–3].However,despite these promising developments,several fundamental challenges hinder their practical implementation and large-scale commercialization.SACs face three major challenges:catalytic activity,stability,and scalable synthesis.Their isolated nature limits multi-electron transfer processes,making reaction kinetics highly sensitive to the coordination environment.To enhance catalytic activity,strategies such as secondary coordination effect,doping,and/or dual-atom configuration can be employed.Stability is another key issue,as single atoms tend to aggregate or undergo oxidation under reaction conditions,leading to performance decay.Strategies like strong metal-support interaction and ligand stabilization can be adopted to improve the durability of SACs.展开更多
By precisely controlling both active sites and their surrounding microenvironments,enzymes catalyze complex transformations with remarkable efficiency and selectivity.This intricate interplay of structure and function...By precisely controlling both active sites and their surrounding microenvironments,enzymes catalyze complex transformations with remarkable efficiency and selectivity.This intricate interplay of structure and function in natural enzymes has inspired the emerging field of precision catalysis,which seeks to similarly modify active site architecture and local environments to enhance catalytic activity and selectivity in nonenzymaticsystems.Precision catalysis aims to enhance activity and selectivity,rivaling natural enzymes while achieving greater atom economy in catalyst design.Among various material platforms,metal-organic frame-works(MOFs)are uniquely positioned to advance precision catalysis due to their modular construction,structural regularity,and synthetic tunability.MOFs are porous crystalline molecular materials built from metal clusters and organic linkers.Their reticular nature enables the rational synthesis of hundreds of thousands of MOFs with diverse topologies and compositions.2 Unlike conventional homogeneous or heterogeneous catalysts,MOFs allow for atomic-level spatial control over the placement of catalytic sites.展开更多
基金financial support from the National Key R&D Program of China(2021YFB3500700)the National Natural Science Foundation of China(22473042,22003016,and 92145302).
文摘The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most significant applications of metal oxides is heterogeneous catalysis,which represents a pivotal technology in industrial production on a global scale.Catalysts serve as the primary enabling agents for chemical reactions,and among the plethora of catalysts,metal oxides including magnesium oxide(MgO),ceria(CeO_(2))and titania(TiO_(2)),have been identified to be particularly effective in catalyzing a variety of reactions[1].Theoretical calculations based on density functional theory(DFT)and a multitude of other quantum chemistry methods have proven invaluable in elucidating the mechanisms of metal-oxide-catalyzed reactions,thereby facilitating the design of high-performance catalysts[2].
文摘Single-atom catalysis has revolutionized heterogeneous catalysis,which offers unparalleled atomic efficiency,well-defined active sites,and unique electronic properties.Unlike traditional nanoparticle catalysts,single-atom catalysts(SACs)maximize metal utilization and exhibit distinct catalytic behaviors due to their atomically dispersed nature.Over the past decade,SACs have demonstrated exceptional performance in various electrochemical and thermocatalytic reactions[1–3].However,despite these promising developments,several fundamental challenges hinder their practical implementation and large-scale commercialization.SACs face three major challenges:catalytic activity,stability,and scalable synthesis.Their isolated nature limits multi-electron transfer processes,making reaction kinetics highly sensitive to the coordination environment.To enhance catalytic activity,strategies such as secondary coordination effect,doping,and/or dual-atom configuration can be employed.Stability is another key issue,as single atoms tend to aggregate or undergo oxidation under reaction conditions,leading to performance decay.Strategies like strong metal-support interaction and ligand stabilization can be adopted to improve the durability of SACs.
文摘By precisely controlling both active sites and their surrounding microenvironments,enzymes catalyze complex transformations with remarkable efficiency and selectivity.This intricate interplay of structure and function in natural enzymes has inspired the emerging field of precision catalysis,which seeks to similarly modify active site architecture and local environments to enhance catalytic activity and selectivity in nonenzymaticsystems.Precision catalysis aims to enhance activity and selectivity,rivaling natural enzymes while achieving greater atom economy in catalyst design.Among various material platforms,metal-organic frame-works(MOFs)are uniquely positioned to advance precision catalysis due to their modular construction,structural regularity,and synthetic tunability.MOFs are porous crystalline molecular materials built from metal clusters and organic linkers.Their reticular nature enables the rational synthesis of hundreds of thousands of MOFs with diverse topologies and compositions.2 Unlike conventional homogeneous or heterogeneous catalysts,MOFs allow for atomic-level spatial control over the placement of catalytic sites.
