The Structural Design of Dual‐Element‐Doped Graphene for Iodine Reduction Reaction: Density Functional Theory Study

Abstract

AbstractDual‐element‐doped graphene has been widely used in the counter electrode due to its enhanced catalytic activity. However, experiments lack a fundamental understanding of the doping effects accounting for the enhanced catalytic activity of dual‐element‐doped graphene. Here, we selected heteroatoms with different electronegativity (e. g., N: 3.0, P: 2.1, Se: 2.4, O: 3.5) based on the C atom with electronegativity of 2.5, then N atoms and heteroatoms co‐doped graphene (N/X‐G, X=P, Se, O) were constructed to investigate the effects of the electronegativity, the doping configuration and position of heteroatoms, the edge structure of graphene on iodine reduction reaction by density functional theory. After a detailed analysis of the electronic structure of N/X‐G, it revealed that the doping of dual‐element could lead to more electrons transfer to the area near heteroatoms, and thus providing more electrons for iodine species. The results of this study indicated that the effects of the dual‐element doping could be divided into three categories, and these principles provide theoretical guidance for further design of the dual‐element‐doped graphene.