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Han et al. J Mater Inf 2023;3:24 Journal of
DOI: 10.20517/jmi.2023.32
Materials Informatics

Research Article Open Access

Regulating the electrocatalytic performance for
nitrogen reduction reaction by tuning the N contents

in Fe @N C (x = 0~4): a DFT exploration
x
3
20-x
Bing Han, Fengyu Li *
School of Physical Science and Technology, Inner Mongolia University, Hohhot 010021, Inner Mongolia, China.

* Correspondence to: Prof. Fengyu Li, School of Physical Science and Technology, Inner Mongolia University, No. 235 Daxue
West Road, Saihan District, Hohhot 010021, Inner Mongolia, China. E-mail: fengyuli@imu.edu.cn

How to cite this article: Han B, Li F. Regulating the electrocatalytic performance for nitrogen reduction reaction by tuning the N
contents in Fe @N C (x = 0~4): a DFT exploration. J Mater Inf 2023;3:24. https://dx.doi.org/10.20517/jmi.2023.32
3 x 20-x
Received: 11 Sep 2023 First Decision: 28 Sep 2023 Revised: 20 Oct 2023 Accepted: 31 Oct 2023 Published: 3 Nov 2023

Academic Editors: Zhongfang Chen, Ming Hu Copy Editor: Pei-Yun Wang Production Editor: Pei-Yun Wang

Abstract
The Haber-Bosch (H-B) process, which is widely used in industry to synthesize ammonia, leads to serious energy
and environment-related issues. The electrochemical nitrogen reduction reaction (eNRR) is the most promising
candidate to replace H-B processes because it is more energy-efficient and environmentally friendly. Atomic-level
catalysts, such as single-atom and double-atom catalysts (SACs and DACs), are of great interest due to their high
atomic utilization and activity. The synergy between the metal atoms and two-dimensional (2D) support not only
modulates the local electronic structure of the catalyst but also controls the catalytic performance. In this article,
we explored the eNRR performance of 2D Fe @N C (x = 0~4), whose structure was based on the experimentally
3 x 20-x
synthesized Ag @C sheet, by means of density functional theory calculations. Through calculations, we found
3 20
that the 2D Fe @N C with Fe site coordinated with four N is a promising eNRR catalyst: the limiting potential is as
3 4 16 2
low as -0.45 V, and the competing hydrogen evolution reaction can be effectively suppressed. Our work not only
confirms that the coordination environment of the metal site is crucial for the electrocatalytic activity but also
provides a new guideline for designing low-cost eNRR catalysts with high efficiency.

Keywords: Electrochemical nitrogen reduction reaction, two dimensions, single-atom and double-atom catalysts,
active site, coordination, density functional theory

© 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,
adaptation, distribution and reproduction in any medium or format, for any purpose, even commercially, as
long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and
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