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Transition-metal-free boron doped SbN monolayer for N2 adsorption and reduction to NH3: A first-principles study.

Authors
  • Chen, Dachang1
  • Chen, Zhiwen2
  • Chen, Lixin2
  • Li, Yi3
  • Xiao, Song3
  • Xiao, Beibei4
  • 1 School of Electrical and Electronic Engineering, Wuhan Polytechnic University, Wuhan 430023, China. Electronic address: [email protected] , (China)
  • 2 Key Laboratory of Automobile Materials, Ministry of Education, School of Materials Science and Engineering, Jilin University, Changchun 130022, China; Department of Materials Science and Engineering, University of Toronto, 184 College Street, Suite 140, Toronto, ON M5S 3E4, Canada. , (Canada)
  • 3 School of Electrical Engineering and Automation, Wuhan University, Wuhan 430072, China. , (China)
  • 4 School of Energy and Power Engineering, Jiangsu University of Science and Technology, Zhenjiang, Jiangsu 212003, China. , (China)
Type
Published Article
Journal
Journal of Colloid and Interface Science
Publisher
Elsevier
Publication Date
Sep 26, 2021
Volume
607
Issue
Pt 2
Pages
1551–1561
Identifiers
DOI: 10.1016/j.jcis.2021.09.026
PMID: 34587530
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

Electrochemical nitrogen reduction reaction (NRR) in ambient condition is an efficient and sustainable method to synthesize NH3. In this work, first-principles study was used to discuss the NRR process on B atom doped SbN monolayer. The adsorption of N2 on B-Sb17N18 and B-S18N17 was calculated including the adsorption energy, adsorption distance, and the charge density difference (CDD). Five different reaction pathways of NRR were taken into consideration and the stability of B-SbN was investigated. The results show that, because the energy of unoccupied orbital in sp3 hybridization of B atom is much lower than that in 2pz orbitals, the adsorption of N2 on B-Sb18N17 shows much larger adsorption energy (-1.01 eV with end-on pattern) compared to that of the adsorption on B-Sb17N18. For five different pathways, the 1, 2, and 4 pathways have a smaller limiting potential of about 0.52 V and the limiting step is: *N2 + H+ + e- → *NNH. The 3 and 5 pathways have a larger limiting potential of 0.57 V with hydrogenation step: *NHNH2 + H+ + e- → *NH2NH2. The B-Sb18N17 is structurally and thermally stable even at 500 K. Our theoretical prediction indicates that B atom substitutionally doped SbN monolayer can be a kind of high-performance metal-free NRR catalyst for NH3 synthetization, and the work provides attempts for designing and exploring 2D metal-free NRR catalysts. Copyright © 2021 Elsevier Inc. All rights reserved.

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