After the synthesis of two‐dimensional(2D)graphene through mechanical exfoliation in 2004,2D nanomaterials have emerged as efficient catalysts for many types of reactions,including heterogeneous catalysis,due to thei...After the synthesis of two‐dimensional(2D)graphene through mechanical exfoliation in 2004,2D nanomaterials have emerged as efficient catalysts for many types of reactions,including heterogeneous catalysis,due to their distinct physicochemical and electronic properties.This review highlights recent progress in the application of 2D materials for selected heterogeneous thermo‐catalytic reactions,with an emphasis on their role as active catalysts or catalyst supports.The catalytic behavior of 2D materials,either as a catalyst or support,in various heterogeneous catalytic reactions,such as Knoevenagel condensation,Suzuki coupling,oxidative dehydrogenation,hydrogenation of nitroarenes,and oxidative desulfurization,is discussed.Particular attention is given to catalyst design strategies involving 2D materials functionalized with metal‐free active sites,as well as hybrid systems incorporating noble and non‐noble metals,although our primary focus is on metal‐free and structurally tunable 2D catalytic platforms.We conclude our discussion with a perspective on present challenges and future recommendations in this fast‐evolving field based on recent state‐of‐the‐art developments.In addition,we provide a critical perspective on current challenges and suggest future directions for the development of cost‐effective,selective,and durable 2D‐based catalysts.展开更多
The high energy density of green synthetic liquid chemicals and fuels makes them ideal for sustainable energy storage and transportation applications.Electroreduction of carbon dioxide(CO_(2))directly into such high v...The high energy density of green synthetic liquid chemicals and fuels makes them ideal for sustainable energy storage and transportation applications.Electroreduction of carbon dioxide(CO_(2))directly into such high value-added chemicals can help us achieve a renewable C cycle.Such electrochemical reduction typically suffers from low faradaic efficiencies(FEs)and generates a mixture of products due to the complexity of controlling the reaction selectivity.This perspective summarizes recent advances in the mechanistic understanding of CO_(2) reduction reaction pathways toward liquid products and the state-of-the-art catalytic materials for conversion of CO_(2) to liquid C1(e.g.,formic acid,methanol)and C2+products(e.g.,acetic acid,ethanol,n-propanol).Many liquid fuels are being produced with FEs between 80%and 100%.We discuss the use of structure-binding energy relationships,computational screening,and machine learning to identify promising candidates for experimental validation.Finally,we classify strategies for controlling catalyst selectivity and summarize breakthroughs,prospects,and challenges in electrocatalytic CO_(2) reduction to guide future developments.展开更多
基金supported by the Joint Funds of the National Natural Science Foundation of China(U24B20201)the National Natural Science Foundation of China(22372007 and 21972010).
文摘After the synthesis of two‐dimensional(2D)graphene through mechanical exfoliation in 2004,2D nanomaterials have emerged as efficient catalysts for many types of reactions,including heterogeneous catalysis,due to their distinct physicochemical and electronic properties.This review highlights recent progress in the application of 2D materials for selected heterogeneous thermo‐catalytic reactions,with an emphasis on their role as active catalysts or catalyst supports.The catalytic behavior of 2D materials,either as a catalyst or support,in various heterogeneous catalytic reactions,such as Knoevenagel condensation,Suzuki coupling,oxidative dehydrogenation,hydrogenation of nitroarenes,and oxidative desulfurization,is discussed.Particular attention is given to catalyst design strategies involving 2D materials functionalized with metal‐free active sites,as well as hybrid systems incorporating noble and non‐noble metals,although our primary focus is on metal‐free and structurally tunable 2D catalytic platforms.We conclude our discussion with a perspective on present challenges and future recommendations in this fast‐evolving field based on recent state‐of‐the‐art developments.In addition,we provide a critical perspective on current challenges and suggest future directions for the development of cost‐effective,selective,and durable 2D‐based catalysts.
基金supported by the Joint Funds of the National Natural Science Foundation of China(U24B20201)National Natural Science Foundation of China(22372007 and 21972010)+1 种基金the Fundamental Research Funds for the Central Universities(JD2427)the SRC Center for Electron Transfer(2021R1A5A1030054)funded by NRF Korea and AI Graduate School Program(RS-2021-II211343).
文摘The high energy density of green synthetic liquid chemicals and fuels makes them ideal for sustainable energy storage and transportation applications.Electroreduction of carbon dioxide(CO_(2))directly into such high value-added chemicals can help us achieve a renewable C cycle.Such electrochemical reduction typically suffers from low faradaic efficiencies(FEs)and generates a mixture of products due to the complexity of controlling the reaction selectivity.This perspective summarizes recent advances in the mechanistic understanding of CO_(2) reduction reaction pathways toward liquid products and the state-of-the-art catalytic materials for conversion of CO_(2) to liquid C1(e.g.,formic acid,methanol)and C2+products(e.g.,acetic acid,ethanol,n-propanol).Many liquid fuels are being produced with FEs between 80%and 100%.We discuss the use of structure-binding energy relationships,computational screening,and machine learning to identify promising candidates for experimental validation.Finally,we classify strategies for controlling catalyst selectivity and summarize breakthroughs,prospects,and challenges in electrocatalytic CO_(2) reduction to guide future developments.
