期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 43, 页码 23699-23708出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c06464
关键词
-
资金
- National Natural Science Foundation of China [21878168]
A single-atom catalyst B/PC6 SAC was constructed and systematically studied for N-2 reduction reaction, showing promising catalytic activity. An external electric field can further enhance the catalytic performance of the B/PC6 SAC.
An electrochemical dinitrogen (N-2) reduction reaction (NRR) under mild conditions has been considered as a promising and sustainable alternative to the conventional Haber-Bosch method. However, searching for an efficient, stable, and low-cost electrocatalyst is still challenging and attractive. Here, based on density functional theory, a single B atom adsorbed on a series of carbon phosphide monolayers [B/PCx single-atom catalysts (SACs), x = 2, 3, 5, and 6] was constructed as metal-free catalysts and their NRR catalytic activities were systematically investigated. Consequently, among the investigated systems, the B/PC6 SAC is identified as the most promising candidate, on which the N-2 molecule can only be sufficiently activated through the enzymatic pathway with a limiting potential of -0.37 V, and importantly, it remains as a stable structure after ab initio molecular dynamics simulations at 300 K. It can be found from the electronic property calculations that the p-orbitals of the B atom have a good degree matching with the p-orbitals of the adsorbed N-2 species, favoring the activation of the N-2 molecule. Besides, both the N-2 adsorption Gibbs free energy and the NRR-limiting overpotential decrease with the increase of the positive electric-field intensity, suggesting that an electric field can be regarded as an effective external stimulus to further improve the catalytic activity of the B/PC6 SAC. This study not only provides an eligible NRR electrocatalyst but also offers a useful tool, that is, applying an external electric field, for the NRR activity enhancement.
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