Issue 16, 2023

Synergetic effect between non-metals and dual metal catalysts for nitrogen reduction reaction

Abstract

Nitrogen reduction reaction (NRR) is an essential process for ammonia synthesis. Currently, such process is overwhelmingly catalyzed with iron-based metal catalysts and still confronts the big challenge of high overpotential when room-temperature electrosynthesis is targeted due to the intrinsic inertness of N[triple bond, length as m-dash]N bond in N2. In this study, dual metal catalysts have been computationally designed and modulated by different non-metals dispersed in a graphene frame. As scanned by density functional theory (DFT) calculations, five candidates, namely Fe2@SN4, Fe2@BN4, Co2@BN4, Co2@PN4 and Ni2@PN4 catalysts, have been identified as promising catalysts with a calculated onset potential of −0.20, −0.27, −0.36, −0.34, and −0.33 V, respectively; more importantly, the competitive hydrogen evolution reaction (HER) can be well suppressed during the NRR. Such excellent catalytic performance origins from two synergetic effects, including the metal–metal and metal–ligands (non-metals) interactions, both of which can promote the electron transfer from d-orbitals of metal atom pair to the anti-bonding orbitals of adsorbed N2 molecules. This can effectively activate the N[triple bond, length as m-dash]N bond, resulting in low NRR onset potential and high NH3 selectivity. The presented theoretical effort advances the theoretical understanding and provides guidance for the rational design of advanced non-precious NRR catalysts with high efficiency and selectivity.

Graphical abstract: Synergetic effect between non-metals and dual metal catalysts for nitrogen reduction reaction

Supplementary files

Article information

Article type
Research Article
Submitted
20 mrt 2023
Accepted
04 jun 2023
First published
14 jun 2023

Inorg. Chem. Front., 2023,10, 4746-4753

Synergetic effect between non-metals and dual metal catalysts for nitrogen reduction reaction

J. Zhang, W. Yang and C. Sun, Inorg. Chem. Front., 2023, 10, 4746 DOI: 10.1039/D3QI00517H

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