A Self-Consistent Framework for Tailored Single-Atom Catalysts in Electrocatalytic Nitrogen Reduction

Mingxin Qin; Lanlan Chen; Wenhua Zhang; Jinlong Yang

doi:10.1021/acs.jpclett.3c03213

A Self-Consistent Framework for Tailored Single-Atom Catalysts in Electrocatalytic Nitrogen Reduction

J Phys Chem Lett. 2024 Feb 1;15(4):1089-1096. doi: 10.1021/acs.jpclett.3c03213. Epub 2024 Jan 23.

Authors

Mingxin Qin¹, Lanlan Chen², Wenhua Zhang^{2

3}, Jinlong Yang²

Affiliations

¹ Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, China.
² Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
³ Laboratory for Chemical Technology, Ghent University, Ghent 9052, Belgium.

PMID: 38261607
DOI: 10.1021/acs.jpclett.3c03213

Abstract

The catalytic activity of single-atom catalysts (SACs) is crucially affected by the actual ligand configurations under the reaction condition; thus, carefully considering the reaction condition is crucial for the theoretical design of SACs. With single metal atoms supported by g-C₃N₄ as a model system, a self-consistent screening framework is proposed for the theoretical design of SACs with respect to the nitrogen reduction reaction (NRR). Pourbaix diagrams are constructed on the basis of various co-adsorption configurations of N₂, H, and OH. Possible stable configurations containing N₂ under the expected reaction condition are considered to obtain the limiting potential of NRR, and the stability of the configuration at the calculated U_L is rechecked. With this framework, AC stacking of double-layer g-C₃N₄-supported Nb and AA stacking and AB stacking of double-layer g-C₃N₄-supported W are predicted to exhibit superior NRR activity with U_L values of -0.36, -0.45, and -0.52 V, respectively. This procedure can be widely applied to the screening of SACs for electrocatalytic reactions.