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Research Article

Single-atom catalysts modified by molecular groups for electrochemical nitrogen reduction

Zengxi Wei1,§, Yuchang Liu1,§, Hongjie Liu1, Shaopeng Wang2,3,4, Minchen Hou5, Liwei Wang2,3,4(), Dong Zhai6, Shuangliang Zhao1, Kefu Yu2,4, Shaolong Zhang5()
Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology and School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, China
School of Marine Sciences, Coral Reef Research Center of China, Guangxi Laboratory on the Study of Coral Reefs in the South China Sea, Guangxi University, Nanning 530004, China
MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials, Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, Nanning 530004, China
Southern Marine Science and Engineering Guangdong Laboratory (Zhuhai), Zhuhai 519080, China
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, China
Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Qingdao 266237, China

§ Zengxi Wei and Yuchang Liu contributed equally to this work.

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Graphical Abstract

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We have screened a series of transition metals single atom catalysts (SACs) in the substrate of g-C3N4 for electrochemical nitrogen reduction reaction (eNRR). The theoretical results exhibited that the W-based SACs can be as a candidate for eNRR.

Abstract

Electrochemical nitrogen reduction reaction (eNRR) is one of the most important chemical reactions for the production of ammonia under ambient environment. However, the lack of in-depth understanding of the structure-activity relationship impedes the development of high-performance catalysts for ammonia production. Herein, the density functional theory (DFT) calculations are performed to reveal the structure–activity relationship for the single-atom catalysts (SACs) supported on g-C3N4, which is modified by molecular groups (i.e., H, O, and OH). The computational results demonstrate that the W-based SACs are beneficial to produce ammonia with a low limiting potential (UL). Particularly, the W-OH@g-C3N4 catalyst exhibits an ultralow UL of −0.22 V for eNRR. And the competitive eNRR selectivity can be identified by the dominant *N2 adsorption free energy than that of *H. Our findings provide a theoretical basis for the synthesis of efficient catalysts to produce ammonia.

Keywords

ammonianitrogen reduction reactionsingle-atom catalysts (SACs)molecular groupsdensity functional theory (DFT) calculations

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Nano Research
Volume 15 Issue 10,
October 2022
Pages 9663-9669
DOI: 10.1007/s12274-022-4550-9
Cite this article:
Wei Z, Liu Y, Liu H, et al. Single-atom catalysts modified by molecular groups for electrochemical nitrogen reduction. Nano Research, 2022, 15(10): 9663-9669. https://doi.org/10.1007/s12274-022-4550-9
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