Enhanced Oxygen Reduction on Graphene via Y5Si3 Electride Substrate: a First-Principles Study

Manipulating the chemical reactivity of graphene toward oxygen reduced reduction (ORR) is of particular interest for both fundamental research and practical application in fuel cell. Deposing graphene on selected substrate provides a structure-intact strategy to enhance its chemical reactivity due to substrate-induced charge and interface effect. Here, we report the graphene deposited on one-dimensional electride Y5Si3 as an effective ORR catalyst in acidic media. Thermodynamic calculations suggest that depositing graphene on electride materials can facilitate the protonation of O-2, which is the rate-determining step based on the four-electron reaction pathway and thus promote the ORR activity. Further electronic calculations reveal that low work function (3.5 eV), superior electrical conductivity and slight charge transfer from substrate to graphene result in the enhanced ORR performance of graphene. These findings shed light on the rational design of ORR catalysts based on graphitic materials and emphasize the critical role of substrates for energy-related electro-chemical reactions.