Precisely designing atomically dispersed catalysts for C-N coupling reactions
Ziheng Zhan, Zihao Wei, Ziteng Zhang, Liping Wang, Weng‐Chon Cheong, Shenghua Li, Wenxing Chen, Siping Pang
Abstract
The electrocatalytic C-N coupling reaction as a green synthesis approach for C-N bond synthesis via electrochemical processes with catalytic assistance. However, inefficient reactant adsorption onto the catalyst surface, competing side reactions, and the complexity and diversity of reaction pathways hinder its widespread application. Atomically dispersed catalysts (ADCs), as an emerging class of catalytic materials, possess precisely defined active sites, high catalytic activity, and enhanced selectivity, thereby enabling efficient electrocatalytic C-N coupling to address these challenges. This review discusses current reaction pathways for converting small molecules (CO<sub>2</sub> as the carbon source, N<sub>2</sub>, NO<sub>2</sub><sup>–</sup>, NO<sub>3</sub><sup>–</sup> as the nitrogen source) into high-value organic nitrogen compounds (urea, amides, oximes, and amino acids) utilizing ADCs. It specifically focuses on the critical steps within electrocatalytic C-N coupling facilitated by these catalysts, encompassing reactant adsorption, transformation and selective hydrogenation of C-/N-intermediates, and the C-N coupling reaction itself. Based on these key steps, design principles for ADCs are proposed. Finally, the synthesis strategies for ADCs—vacancy engineering, confinement strategies, and alloying—are examined, alongside the mechanisms by which they enhance catalytic activity and selectivity.