期刊
JOURNAL OF ENERGY CHEMISTRY
卷 66, 期 -, 页码 628-634出版社
ELSEVIER
DOI: 10.1016/j.jechem.2021.09.020
关键词
Nitrogen reduction; Electrocatalysis; Intermediate stabilization strategy; Density functional theory
资金
- National Natural Science Foundation of China (NSFC) [51972312, U20A20242]
- Liaon-ing Provincial Natural Science Foundation of China [2020-MS-003]
This study proposes a new strategy to improve the performance of electrocatalytic nitrogen reduction reaction by using catalysts with frustrated Lewis pairs, identifying promising candidates with low limiting potentials and high selectivity, offering a new opportunity for accelerated and cost-effective ammonia synthesis through electrocatalysis.
Electrocatalytic nitrogen reduction reaction (eNRR) with sustainable energy under ambient conditions represents an attractive approach to producing ammonia, but the design of the-state-of-the-art electrocatalyst with high efficiency and selectivity still faces formidable challenges. In contrast to traditional eNRR catalyst design strategies focusing on N N triple bond activation, we herein theoretically proposed an alternative strategy to improve eNRR performance via stabilizing the N2H* intermediate using catalysts with the frustrated Lewis pairs (FLPs), i.e., transition metal (TM) atoms and boron (B) atom codoped 2D black phosphorus (TM-B@BP). Our density functional theory (DFT) results reveal that the TM atom donates electrons to the adsorbed N-2 molecule, while B atom provides empty orbital to stabilize the adsorption of N2H* intermediate. This framework successfully identifies five promising candidates (i.e., Ti-B@BP, V-B@BP, Cr-B@BP, Mn-B@BP and Fe-B@BP) with low theoretical limiting potentials (-0.60, -0.41, -0.45, -0.43 and -0.50 V, respectively) and high selectivity for eNRR. We believe that the intermediate stabilization strategy introduced in current work offers a new opportunity to achieve accelerated and cost-effective ammonia synthesis with electrocatalysis. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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