期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 607, 期 -, 页码 1551-1561出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.09.026
关键词
Nitrogen reduction reaction (NRR); First-principles study; B doping; SbN monolayer; Transition-metal-free catalyst
资金
- China National Postdoctoral Program for Innovative Talents [BX2021224]
- National Natural Science Foundation of P. R. China [51977159]
The study explored the electrochemical nitrogen reduction reaction (NRR) on B atom doped SbN monolayer using first-principles approach, revealing the adsorption behavior of N-2 and different reaction pathways. Results showed that B-Sb18N17 is a promising high-performance catalyst for NH3 synthesis and remains structurally stable at elevated temperatures.
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 N-2 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 sp(3) hybridization of B atom is much lower than that in 2pz orbitals, the adsorption of N-2 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: *N-2 + 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. (C) 2021 Elsevier Inc. All rights reserved.
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