期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 45, 页码 19308-19315出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c09527
关键词
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资金
- National Key Research and Development Program of China [2018YFA0208603]
- National Natural Science Foundation of China (NSFC) [22063001, 21633006, 21562002, 21962002]
- Anhui Initiative in Quantum Information Technologies [AHY090200]
- DNL Cooperation Fund CAS [DNL201913]
- Funding Project for Academic/Technical Leaders of Jiangxi Province [20172BCB22021]
- NSF of Jiangxi Provincial Education Department [GJJ190756]
- Supercomputing Center of University of Science and Technology of China
Developing efficient single-atom catalysts (SACs) for nitrogen fixation is of great importance while remaining a great challenge. The lack of an effective strategy to control the polarization electric field of SACs limits their activity and selectivity. Here, using first-principles calculations, we report that a single transition metal (TM) atom sandwiched between hexagonal boron nitride (h-BN) and graphene sheets (namely, BN/TM/G) acts as an efficient SAC for the electrochemical nitrogen reduction reaction (NRR). These sandwich structures realize stable and tunable interfacial polarization fields that enable the TM atom to donate electrons to a neighboring B atom as the active site. As a result, the partially occupied p(z) orbital of a B atom can form B-to-N pi-back bonding with the antibonding state of N-2, thus weakening the N N bond. The not-strong-not-weak electric field on the h-BN surface further promotes N-2 adsorption and activation. The NRR catalytic activity of the BN/TM/G system is highly correlated with the degree of positively polarized charges on the TM atom. In particular, BN/Ti/G and BN/V/G are identified as promising NRR catalysts with high stability, offering excellent energy efficiency and suppression of the competing hydrogen evolution reaction.
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