作者：

Haoyu Wang¹, Oleg V. Prezhdo²*, Lai Xu¹*

单位：

¹State Key Laboratory of Bioinspired Interfacial Materials Science, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China.

²Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque, New Mexico 87106, United States.

摘要：

Electrocatalytic urea production through C−N coupling offers a sustainable alternative to traditional energy-intensive processes; however, its practical implementation is still limited by thermodynamically unfavorable pathways and slow C− N coupling kinetics. We design systematically a series of twisted two-dimensional heterostructures composed of BCN and MXenes, denoted as M2CO/BCN (M = Ti, V, Cr), with six representative rotation angles (0°, 10.89°, 49.11°, 60°, 70.89°, and 109.11°). Density functional theory calculations reveal that interfacial twisting effectively modulates charge redistribution and electronic coupling, thereby promoting CO and NO activation. Thermodynamic analyses combined with constrained ab initio molecular dynamics simulations demonstrate that twisting markedly reduces both the free energy variation and the kinetic barriers associated with the C−N coupling step. As a result, V₂CO/BCN-109.11° exhibits the lowest reaction potential of −0.23 V. Our findings establish interfacial twisting as an effective strategy for simultaneously optimizing thermodynamics and kinetics in electrocatalytic urea synthesis. Finally, we apply the Sure Independence Screening and Sparsifying Operator (SISSO) approach to identify a physically interpretable descriptor that quantitatively correlates twist-induced structural factors with catalytic performance, providing a key insight into the structure−activity relationship.

影响因子：

15.6

分区情况：

一区

链接：

https://pubs.acs.org/doi/10.1021/jacs.6c04758