Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and Electrocatalysis with Model Molecules  

作　　者：Wei Guo Linhui Yu Ling Tang Yan Wan Yangming Lin 

机构地区：[1]CAS Key Laboratory of Design and Assembly of Functional Nanostructures,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,People’s Republic of China [2]Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials,Xiamen Institute of Rare Earth Materials,Haixi Institute,Chinese Academy of Sciences,Xiamen 361021,People’s Republic of China [3]State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,People’s Republic of China [4]Institute of Urban Environment,Chinese Academy of Sciences,Xiamen 361021,People’s Republic of China

出　　处：《Nano-Micro Letters》2024年第7期74-97,共24页纳微快报（英文版）

基　　金：We are grateful for financial support from the“Hundred Talents Program”of the Chinese Academy of Sciences and the“Young Talents Training Program”of the Shanghai Branch of the Chinese Academy of Sciences.We acknowledge the financial support from the National Science Youth Foundation of China(22202205);Xiamen City Natural Science Foundation of China(3502Z20227256);Fujian Provincial Natural Science Foundation of China(2022J01502).

摘　　要：Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Over the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms.However,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods.In this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon catalysis.Using both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically studied.Combined with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular level.Furthermore,the outlook of model carbon catalysis has also been proposed in this work.

关 键 词：Metal-free carbon catalysts Model catalyst ELECTROCATALYSIS Active site Reaction mechanisms 

分 类 号：O643.36[理学—物理化学]