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

• DOI: 10.1021/acs.jpclett.1c02432
• Publication Date: 2021-08-25T20:12:35Z
• Authors: Qian Dang; Shaobin Tang; Tianyong Liu; Xiaokang Li; Xijun Wang; Wenhui Zhong; Yi Luo; Jun Jiang
• Keywords: Spin states; Basal plane

The electrocatalytic activity of transition-metal (TM)-based catalysts is correlated with the spin states metal atoms. However, developing a way to manipulate remains great challenge. Using first-principles calculations, we first report crucial role exposed Mo atoms around an S-vacancy in dinitrogen reduction reaction on defective MoS2 nanosheets and propose novel strategy for regulating electronic moments by tuning single-atom promoter (SAP). Single TM adsorbed basal plane serve as SAPs via noncontact interaction active site, inducing significant polarization that promotes N2 adsorption activation. Interestingly, changing only site atom, are able change over wide range tunable values. can be tuned largely improve catalytic toward NH3.