期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 12, 期 34, 页码 8355-8362出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c02432
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资金
- National Key Research and Development Program of China [2018YFA0208603]
- National Natural Science Foundation of China (NSFC) [22063001, 21963007, 21962002]
- Anhui Initiative in Quantum Information Technologies [AHY090200]
- DNL Cooperation Fund CAS [DNL201913]
The study demonstrates that manipulating the spin moments of metal atoms in MoS2 nanosheets through tuning a single-atom promoter can significantly enhance the electrocatalytic activity of the dinitrogen reduction reaction. By changing the adsorption site of the single transition-metal atom, the spin moments of the metal atom can be altered over a wide range, improving the catalytic efficiency towards the reduction of N-2 to NH3.
The electrocatalytic activity of transition-metal (TM)-based catalysts is correlated with the spin states of metal atoms. However, developing a way to manipulate spin remains a great challenge. Using first-principles calculations, we first report the crucial role of the spin of exposed Mo atoms around an S-vacancy in the electrocatalytic dinitrogen reduction reaction on defective MoS2 nanosheets and propose a novel strategy for regulating the electronic spin moments by tuning a single-atom promoter (SAP). Single TM atoms adsorbed on a defective MoS2 basal plane serve as SAPs via a noncontact interaction with an exposed Mo active site, inducing a significant spin polarization that promotes N-2 adsorption and activation. Interestingly, by changing only the adsorption site of the TM atom, we are able to change the spin moments of the Mo atom, over a wide range of tunable values. The spin moments can be tuned to largely improve the catalytic activity of MoS2 toward the reduction of N-2 to NH3.
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