Electrocatalytic Reduction of N2Using Metal-Doped Borophene

Lu Xu; Li Ming Yang; Eric Ganz

doi:10.1021/acsami.0c20553

Electrocatalytic Reduction of N₂Using Metal-Doped Borophene

Lu Xu, Li Ming Yang, Eric Ganz

Physics and Astronomy (Twin Cities)

Research output: Contribution to journal › Article › peer-review

87 Scopus citations

Abstract

Ammonia synthesis is an essential process in chemistry and industry. However, it is limited by the lack of efficient catalysts and high energy costs. Developing highly efficient systems for ammonia synthesis is an important and long-standing challenge. In this paper, a large class of metal atoms (including 3d/4d transition metals and main group metals) anchored onto borophene have been studied as single atom catalysts for ammonia synthesis. After comprehensive computational screening and systematic evaluation, four candidates stand out. We predict that Mo, Mn, Tc, and Cr@BM-β12 will have superior performance for catalytic reduction of N2 to NH3 with low limiting potentials of -0.26, -0.32, -0.38, and -0.48 V, respectively. Furthermore, we studied the activity of the competitive HER on M@BM-β12. The results implied that the two materials Mo@BM-β12 and Mn@BM-β12 showed HER suppression. These properties exceed most currently reported nitrogen reduction reaction electrocatalysts. Our results suggest the possibility of efficient electrochemical reduction of N2 to NH3 in a lower energy process.

Original language	English (US)
Pages (from-to)	14091-14101
Number of pages	11
Journal	ACS Applied Materials and Interfaces
Volume	13
Issue number	12
DOIs	https://doi.org/10.1021/acsami.0c20553
State	Published - Mar 31 2021

Bibliographical note

Funding Information:
L.X. and L.-M.Y. gratefully acknowledge support from the National Natural Science Foundation of China (22073033, 21873032, 21673087, and 21903032), startup fund (2006013118 and 3004013105) from the Huazhong University of Science and Technology, and the Fundamental Research Funds for the Central Universities (2019kfyRCPY116). The authors thank the Minnesota Supercomputing Institute (MSI) at the University of Minnesota for supercomputing resources. Additional work was carried out at LvLiang Cloud Computing Center of China, and some calculations were performed on TianHe-2.

Publisher Copyright:
©

Keywords

borophene
density functional theory
electrocatalytic nitrogen reduction reaction
high-throughput screening
single-atom catalyst

PubMed: MeSH publication types

Journal Article

Publisher link

10.1021/acsami.0c20553

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title = "Electrocatalytic Reduction of N2Using Metal-Doped Borophene",

abstract = "Ammonia synthesis is an essential process in chemistry and industry. However, it is limited by the lack of efficient catalysts and high energy costs. Developing highly efficient systems for ammonia synthesis is an important and long-standing challenge. In this paper, a large class of metal atoms (including 3d/4d transition metals and main group metals) anchored onto borophene have been studied as single atom catalysts for ammonia synthesis. After comprehensive computational screening and systematic evaluation, four candidates stand out. We predict that Mo, Mn, Tc, and Cr@BM-β12 will have superior performance for catalytic reduction of N2 to NH3 with low limiting potentials of -0.26, -0.32, -0.38, and -0.48 V, respectively. Furthermore, we studied the activity of the competitive HER on M@BM-β12. The results implied that the two materials Mo@BM-β12 and Mn@BM-β12 showed HER suppression. These properties exceed most currently reported nitrogen reduction reaction electrocatalysts. Our results suggest the possibility of efficient electrochemical reduction of N2 to NH3 in a lower energy process. ",

keywords = "borophene, density functional theory, electrocatalytic nitrogen reduction reaction, high-throughput screening, single-atom catalyst",

author = "Lu Xu and Yang, {Li Ming} and Eric Ganz",

note = "Funding Information: L.X. and L.-M.Y. gratefully acknowledge support from the National Natural Science Foundation of China (22073033, 21873032, 21673087, and 21903032), startup fund (2006013118 and 3004013105) from the Huazhong University of Science and Technology, and the Fundamental Research Funds for the Central Universities (2019kfyRCPY116). The authors thank the Minnesota Supercomputing Institute (MSI) at the University of Minnesota for supercomputing resources. Additional work was carried out at LvLiang Cloud Computing Center of China, and some calculations were performed on TianHe-2. Publisher Copyright: {\textcopyright} ",

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T1 - Electrocatalytic Reduction of N2Using Metal-Doped Borophene

AU - Xu, Lu

AU - Yang, Li Ming

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N1 - Funding Information: L.X. and L.-M.Y. gratefully acknowledge support from the National Natural Science Foundation of China (22073033, 21873032, 21673087, and 21903032), startup fund (2006013118 and 3004013105) from the Huazhong University of Science and Technology, and the Fundamental Research Funds for the Central Universities (2019kfyRCPY116). The authors thank the Minnesota Supercomputing Institute (MSI) at the University of Minnesota for supercomputing resources. Additional work was carried out at LvLiang Cloud Computing Center of China, and some calculations were performed on TianHe-2. Publisher Copyright: ©

PY - 2021/3/31

Y1 - 2021/3/31

N2 - Ammonia synthesis is an essential process in chemistry and industry. However, it is limited by the lack of efficient catalysts and high energy costs. Developing highly efficient systems for ammonia synthesis is an important and long-standing challenge. In this paper, a large class of metal atoms (including 3d/4d transition metals and main group metals) anchored onto borophene have been studied as single atom catalysts for ammonia synthesis. After comprehensive computational screening and systematic evaluation, four candidates stand out. We predict that Mo, Mn, Tc, and Cr@BM-β12 will have superior performance for catalytic reduction of N2 to NH3 with low limiting potentials of -0.26, -0.32, -0.38, and -0.48 V, respectively. Furthermore, we studied the activity of the competitive HER on M@BM-β12. The results implied that the two materials Mo@BM-β12 and Mn@BM-β12 showed HER suppression. These properties exceed most currently reported nitrogen reduction reaction electrocatalysts. Our results suggest the possibility of efficient electrochemical reduction of N2 to NH3 in a lower energy process.

AB - Ammonia synthesis is an essential process in chemistry and industry. However, it is limited by the lack of efficient catalysts and high energy costs. Developing highly efficient systems for ammonia synthesis is an important and long-standing challenge. In this paper, a large class of metal atoms (including 3d/4d transition metals and main group metals) anchored onto borophene have been studied as single atom catalysts for ammonia synthesis. After comprehensive computational screening and systematic evaluation, four candidates stand out. We predict that Mo, Mn, Tc, and Cr@BM-β12 will have superior performance for catalytic reduction of N2 to NH3 with low limiting potentials of -0.26, -0.32, -0.38, and -0.48 V, respectively. Furthermore, we studied the activity of the competitive HER on M@BM-β12. The results implied that the two materials Mo@BM-β12 and Mn@BM-β12 showed HER suppression. These properties exceed most currently reported nitrogen reduction reaction electrocatalysts. Our results suggest the possibility of efficient electrochemical reduction of N2 to NH3 in a lower energy process.

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