Mixture screening strategy of efficient transition metal heteronuclear dual-atom electrocatalysts toward nitrogen fixation

作者：Zhu, Zhouhao; Chen, Mengshan; Sun, Mingyuzhi; Wang, Jinhu; Zhou, Yingtang^*; Li, Xibao^*; Tao, Hengcong^*

来源：Physical Chemistry Chemical Physics, 2022, 24(43): 26776-26784.

DOI：10.1039/d2cp04302e

• OXYGEN REDUCTION
• SINGLE-ATOM
• AMMONIA
• N-2
• CATALYSTS
• GRAPHENE
• MECHANISM
• CO

To rapidly design nitrogen reduction reaction (NRR) electrocatalysts with superior activity and selectivity is a great challenge. Herein, we propose a simple mixture strategy including three screening steps and a descriptor to predict NRR electrocatalysts with outstanding activity and selectivity based on density functional theory (DFT). Twenty-eight candidate transition-metal dimers anchored on nitrogen-doped graphene were systematically investigated through our mixture strategy. The results show that VRu-NC exhibits a high NRR activity and suppression of the competitive hydrogen evolution reaction (HER) following the mixed mechanism with a favorable limiting potential (U-L) of -0.21 V. Finally, the mechanism of the catalytic reaction pathway was investigated according to the profile of atomic orbitals and electronic properties. This work proposes a feasible strategy for rapid screening of the high-performance of double atomic electrocatalysts with excellent activity and selectivity for the NRR.

• 单位
  南昌航空大学