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Pei et al. J Mater Inf 2023;3:26 Journal of
DOI: 10.20517/jmi.2023.35
Materials Informatics

Research Article Open Access

Computational design of spatially confined triatomic
catalysts for nitrogen reduction reaction

2
1,#
1
1
1
1
Wei Pei 1,#,* , Wenya Zhang , Xueke Yu , Lei Hou , Weizhi Xia , Zi Wang , Yongfeng Liu , Si Zhou 3,* ,
1,*
Yusong Tu , Jijun Zhao 2
1
College of Physics Science and Technology, Yangzhou University, Yangzhou 225009, Jiangsu, China.
2
Key Laboratory of Structural Analysis for Industrial Equipment, Dalian University of Technology, Dalian 116024, Liaoning, China.
3
School of Physics, South China Normal University, Guangzhou 510631, Guangdong, China.
#
Authors contributed equally.
* Correspondence to: Dr. Wei Pei, Prof. Yusong Tu, College of Physics Science and Technology, Yangzhou University, No.180
Siwangting Road, Yangzhou 225009, Jiangsu, China. E-mail: pwei@yzu.edu.cn; ystu@yzu.edu.cn; Prof. Si Zhou, School of
Physics, South China Normal University, No. 378 Huanxi Road, Guangzhou 510631, Guangdong, China. E-mail:
sizhou@m.scnu.edu.cn
How to cite this article: Pei W, Zhang W, Yu X, Hou L, Xia W, Wang Z, Liu Y, Zhou S, Tu Y, Zhao J. Computational design of
spatially confined triatomic catalysts for nitrogen reduction reaction. J Mater Inf 2023;3:26. https://dx.doi.org/10.20517/jmi.
2023.35
Received: 4 Nov 2023 First Decision: 24 Nov 2023 Revised: 3 Dec 2023 Accepted: 18 Dec 2023 Published: 21 Dec 2023
Academic Editors: Fengyu Li, Xingjun Liu Copy Editor: Pei-Yun Wang Production Editor: Pei-Yun Wang

Abstract
The electrocatalytic process of nitrogen reduction reactions (NRR) offers a promising approach towards achieving
sustainable ammonia production, acting as an environmentally friendly replacement for the conventional Haber-
Bosch method. Density functional theory calculations have been utilized to design and investigate a set of catalysts
known as triple-atom catalysts (TACs) for electrochemical NRR, which are supported on graphite-C N
3 3
nanosheets. Herein, we have systematically evaluated these TACs using stringent screening to assess their
catalytic performance. Among the candidates, supported Pt , Re , and Ru trimers emerged as highly active with
3 3 3
decent selectivity, involving a limiting potential range of -0.35~-0.11 V. According to analysis of electronic
properties, we determined that high NRR activity stems from the d-π* electron-accepting and -donating
mechanism. Significantly, the correlation between chemical activity of TACs and electronic structure was
established as a pivotal physical parameter, which has led to the conclusion that we can precisely control the
catalytic behavior of transition metal trimer clusters by selecting appropriate metal elements and designing
moderate cluster-substrates interactions. In summary, these theoretical studies not only enhance our
understanding of how catalytic properties are governed by metal-support interactions, regulating stability, activity,

© The Author(s) 2023. Open Access This article is licensed under a Creative Commons Attribution 4.0
International License (https://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, sharing,
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