Autonomous Exploitation of Reaction Pathways for Electrochemical C–N Coupling on Single-Atom Catalysts

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-12-18 DOI:10.1021/acscatal.4c05751
Junjie Pan, Haowen Ding, Xinzhe Yang, Xianhui Liang, Shanglin Wu, Mingzheng Zhang, Shunning Li, Shisheng Zheng, Feng Pan
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Abstract

Electrochemical C–N coupling between CO2 and N-containing small molecules is a promising strategy to close both the carbon and nitrogen loops to support the establishment of a net-zero carbon economy. However, the intricate reaction network and the contentious C–N coupling mechanism hinder the development of efficient electrocatalysts for industrial applications. Herein, we develop a graph-based approach to enable autonomous analysis of the C–N coupling mechanism for coreduction of CO2 and NO3 on single-atom catalysts (SACs). 1400 potential intermediates and 2490 C–N coupling modes are investigated based on the Cu-N4-C prototypical catalyst. We demonstrate that N-containing species with a higher reduction degree are more likely to undergo C–N coupling and the initial coupling of the C–N bond tends to occur on CO2. It is revealed that the hydrogenation energies of *NH2 and CO2, as well as their coupling energies, can serve as key indicators for catalyst recommendation. Using this approach, SACs with Mo, W, or Sb metal centers are identified as promising electrocatalysts for C–N coupling. This work presents a paradigm for automatically exploring the mechanisms of complex electrocatalytic reactions and offers a strategy for predicting highly active and selective SACs.

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ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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