题目：

Design of Boron and Transition Metal Embedded Two-Dimensional Porous Carbon Nitride for Electrocatalytic Synthesis of Urea

作者：

Xin Cao¹, Dewei Zhang¹, Yongqi Gao¹, Oleg V. Prezhdo²*, Lai Xu¹*

单位：

¹Institute of Functional Nano & Soft Materials (FUNSOM) , Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Jiangsu Key Laboratory for CarbonBased Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices,Soochow University, Suzhou 215123 Jiangsu, People’s Republic of China

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

摘要：

Electrocatalytic coupling of CO and N₂ to synthesize urea under ambient conditions is considered a promising strategy to replace traditional industrial technology. It is crucial to find efficient electrocatalysts that can adsorb and activate N₂ and promote the C–N coupling reaction. Herein, a new two-dimensional porous carbon nitride material with multiactive sites is designed, in which boron and transition metal are embedded. Through a series of screening, B₂Cr₂, B₂Mn₂, and B₂Os₂ are predicted to be potential electrocatalysts for urea synthesis. Mechanistic studies are performed on bidentate metal–metal and metal–boron sites, and both NCON and CO mechanisms are explored. The electronic structure analysis shows that there is a strong N₂ chemical adsorption within the bidentate site and that the N≡N bond is significantly activated. A new mechanism where free CO is inserted for C–N coupling within the two-dimensional porous structure is proposed.

影响因子：

16.383

分区情况：

一区

链接：

https://pubs.acs.org/doi/10.1021/jacs.3c12017