(269c) Unravelling Hydrogenation Barriers for CO2 Reduction on Nitrogen Doped Zigzag Edges of Graphene

We have used first principles quantum chemistry methods including cluster-continuum solvation modeling and the growing string method to study reaction pathways for CO₂ reduction on cluster models for nitrogen doped zigzag edges of graphene. Our motivation was to better understand the viability of fundamental pathways classified as sequential proton and electron transfers, hydrogen atom transfers, and proton-coupled hydride transfers that would convert CO₂ into CO, formate, and other more reduced products. We analyzed the degree that local solvation environments (i.e. explicit solvent molecules and the proximity of electrolyte ions) would impact the relative energetics of these pathways. This work provides an atomic scale elucidation of energetically viable hydrogenation pathways for the design of renewable energy catalysts.