题目：

Design of a Four-Atom Cluster Embedded in Carbon Nitride for Electrocatalytic Generation of Multi-Carbon Products

作者：

Dewei Zhang¹, Oleg V. Prezhdo²*, and Lai Xu¹*

单位：

¹Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon Based Functional Materials & Devices, Soochow University, Suzhou 215123, P. R. China.

²Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States.

摘要：

The development of efficient and stable catalysts for the electrocatalytic CO₂ and CO reduction reactions (CORR) is under active investigation, but the problems of poor selectivity and low efficiency for C₂ products still exist. We design a two-dimensional carbon nitride material (C₅N₂H₂) that contains an eight N-atom structure capable of coordinating four-metal atom clusters and supporting simultaneously two carbon oxide molecules needed for the C₂ coupling. The designed material has excellent electrical conductivity and stability. After high-throughput screening of catalytic performance of multiple four-metal clusters embedded into the framework, we systematically investigate the CORR process of 11 candidates. We find that Cu₄-C₅N₂H₂ has superior selectivity and low limiting potential for generating ethylene, while Cu₂Zn₂-C₅N₂H₂ is selective and efficient to synthesize ethanol. Further, we discover a novel type of descriptor related to 2D material flexibility to evaluate the potential-determining step for generating ethylene. Our report both broadens the possibilities for few-atom CO reduction and demonstrates a novel substrate flexibility-related descriptor to predict the catalytic performance of materials.

影响因子：

16.383

分区情况：

一区

链接：

https://pubs.acs.org/doi/10.1021/jacs.3c01561