Two-Dimensional Ordered Double-Transition Metal Carbides for the Electrochemical Nitrogen Reduction Reaction

Rong Zhao; Yongting Chen; Hui Xiang; Yunfeng Guan; Chenfan Yang; Qin Zhang; Yanjun Li; Ye Cong; Xuanke Li

doi:10.1021/acsami.2c19911

Two-Dimensional Ordered Double-Transition Metal Carbides for the Electrochemical Nitrogen Reduction Reaction

ACS Appl Mater Interfaces. 2023 Feb 8;15(5):6797-6806. doi: 10.1021/acsami.2c19911. Epub 2023 Jan 27.

Authors

Rong Zhao¹, Yongting Chen¹, Hui Xiang¹, Yunfeng Guan¹, Chenfan Yang², Qin Zhang¹, Yanjun Li¹, Ye Cong¹, Xuanke Li¹

Affiliations

¹ School of Chemistry and Chemical Engineering, Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, Wuhan University of Science and Technology, Wuhan430081, China.
² Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, College of Materials Science and Engineering, Hunan University, Changsha410082, China.

PMID: 36705631
DOI: 10.1021/acsami.2c19911

Abstract

The electrochemical nitrogen reduction reaction (NRR) provides a green and sustainable strategy as an alternative to the Haber-Bosch process. The development of electrocatalysts with low overpotential, high selectivity, and fast reaction kinetics remains a significant challenge. Here, density functional theory computations are carried out to systematically predict the prospect of 18 two-dimensional (2D) ordered double-transition metal carbides (MXenes) as NRR electrocatalysts. Our results revealed that the basal plane of Mo₂Nb₂C₃ MXene exhibited the most outstanding catalytic activity while effectively suppressed the hydrogen evolution reaction with an overpotential of 0.48 V. The exposed Mo₃ moiety moderately regulating the electron transfer between reaction intermediates is answerable for the high activity. Finally, our finding broadens the horizon of 2D materials as NRR electrocatalysts.

Keywords: 2D materials; DFT calculations; MXene; catalytic mechanism; electrochemistry; nitrogen reduction reaction.