Theoretical Screening of Single-Atom-Embedded MoSSe Nanosheets for Electrocatalytic N-2 Fixation

作者：Li, Lei; Li, Baihai; Guo, Qiuyan; Li, Bo

来源：Journal of Physical Chemistry C, 2019, 123(23): 14501-14507.

DOI：10.1021/acs.jpcc.9b02657

• TOTAL-ENERGY CALCULATIONS
• AMMONIA-SYNTHESIS
• RECENT PROGRESS
• NITROGEN
• TRANSITION
• REDUCTION
• DINITROGEN
• MO

The NH3 synthesis from N-2 electrochemical reduction under mild conditions is a great challenge. In this study, we investigated a series of transition-metal-embedded MoSSe nanosheets with S or Se vacancy based on the density functional theory calculations. Our results revealed that Mo-embedded MoSSe with S vacancy exhibits the best catalytic performance following the alternating mechanism. The potential-limiting step is the first hydrogenation of the adsorbed N-2 with a barrier of 0.49 eV. The relatively low Delta G of 0.58 eV for NH3 desorption allows the rapid removal of the products from the catalyst. The high stability of the adsorbed N2H species implies the great catalytic activity of the Mo-embedded MoSSe. By comparing the adsorption strength between single H atom and N-2 molecule on the active site, the Mo-doped MoSSe possesses a much higher selectivity on nitrogen reduction reaction. Our research may provide insightful ideas for the efficient electrochemical reduction of N-2 to NH3 in ambient conditions.

• 单位
  中国科学院宁波材料技术与工程研究所; 电子科技大学