Regulating Electronic Spin Moments of Single-Atom Catalyst Sites via Single-Atom Promoter Tuning on S-Vacancy MoS2 for Efficient Nitrogen Fixation

被引:80
作者
Dang, Qian [1 ]
Tang, Shaobin [1 ]
Liu, Tianyong [1 ]
Li, Xiaokang [1 ]
Wang, Xijun [2 ]
Zhong, Wenhui [3 ]
Luo, Yi [2 ]
Jiang, Jun [2 ]
机构
[1] Gannan Normal Univ, Key Lab Organo Pharmaceut Chem Jiangxi Prov, Ganzhou 341000, Peoples R China
[2] Univ Sci & Technol China, Sch Chem & Mat Sci, CAS Ctr Excellence Nanosci, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
[3] Qufu Normal Univ, Sch Chem & Chem Engn, Qufu 273165, Shandong, Peoples R China
基金
中国国家自然科学基金;
关键词
REDUCTION; EVOLUTION; IDENTIFICATION; MONOLAYER; OXIDATION; AMMONIA;
D O I
10.1021/acs.jpclett.1c02432
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:8355 / 8362
页数:8
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