Issue

Vol. 16 (2024)

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

https://doi.org/10.1007/s40820-023-01262-8
Wei Guo
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
Linhui Yu
Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, People’s Republic of China
Ling Tang
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
Yan Wan
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
Yangming Lin
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

Corresponding Author: Yangming Lin

xmlinyangming@fjirsm.ac.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 125

Abstract

Metal-free carbon, as the most representative heterogeneous metal-free catalysts, have received considerable interests in electro- and thermo-catalytic reactions 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 summarize 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.


Highlights:
1 Mechanistic understandings of metal-free carbon thermocatalysis and electrocatalysis from the viewpoint of model method are summarized.
2 Active sites and reaction mechanisms are discussed with a focus on in-situ techniques and 2D structure–activity relationships.
3 The real contribution of each alien species, defect and edge configuration to catalytic reactions are systematically highlighted at a molecular level.

Keywords

Metal-free carbon catalysts Model catalyst Electrocatalysis Active site Reaction mechanisms
Guo, Wei, Linhui Yu, Ling Tang, Yan Wan, and Yangming Lin. 2024. “Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and Electrocatalysis With Model Molecules”. Nano-Micro Letters 16 (February):125. https://doi.org/10.1007/s40820-023-01262-8.
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