Unravelling the 2e- ORR Activity Induced by Distance Effect on Main-Group Metal InN4 Surface Based on First Principles

Peng Li; Jiawen Xu; Yaqiong Su

doi:10.3390/molecules27227720

Unravelling the 2e^- ORR Activity Induced by Distance Effect on Main-Group Metal InN₄ Surface Based on First Principles

Molecules. 2022 Nov 9;27(22):7720. doi: 10.3390/molecules27227720.

Authors

Peng Li¹, Jiawen Xu², Yaqiong Su¹

Affiliations

¹ School of Chemistry, Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, State Key Laboratory of Electrical Insulation and Power Equipment, Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education, Xi'an Jiaotong University, Xi'an 710049, China.
² General Research Institute of Engineering of Gotion High-Tech, Baohe District, Hefei 230041, China.

Abstract

The p-electron-dominated main-group metals (Sb, Se, In, etc.) have recently been reported to possess excellent oxygen reduction reaction (ORR) activity by means of heteroatom doping into graphene. However, on these main group metal surfaces, other approaches especially the distance effect to modulate catalytic activity are rarely involved. In this work, the origin of excellent 2e^- ORR catalytic activity of graphene-supported InN₄ moiety by tuning the distance between metallic In atoms is thoroughly investigated by employing the first-principles calculations. Our DFT calculations show that the 2e^- ORR catalytic activity strongly depends on the crystal orbital Hamilton population (COHP) between In and O atoms. This work is useful for the rational design of main group metal single atom electrocatalysts.

Keywords: 2e− ORR; distance effect; main group metal; metal-N doped graphene.

Grants and funding

This research was funded by the “Young Talent Support Plan” of Xi’an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018).