单原子金属-氮-石墨烯催化 CO2 液相电化学还原的理论模拟

单原子金属-氮-石墨烯材料(M-N-Gra)被认为是理想的CO2电化学还原反应的催化剂，为替代贵金属基催化材料提供了新策略. CO2电化学还原反应发生在M-N-Gra电极/电解质溶液之间的固液界面上，然而固液界面的行为十分复杂，该反应的机理尚不明确. 本研究拟采用密度泛函理论结合分子动力学模拟，开展M-N-Gra电极/电解质溶液界面上的CO2还原化学反应机制的研究，探究在接近真实固液电化学界面反应条件下的固液界面特性、催化活性中心结构和催化反应动力学，研究中着重处理水、水中物种以及电极电势对催化反应的影响和调控，以期深入理解其反应机理，并探究合适反应条件和催化剂结构，为设计基于M-N-Gra的CO2RR催化剂奠定理论基础.

Single atom metal-nitrogen-graphene materials (M-N-Gra) are excellent promising catalysts for CO2 electrochemical reduction reaction (CO2RR), providing new strategy for replacing precious-metal catalysts. The CO2RR occurs at the solid electrode/liquid electrolyte interface between the M-N-Gra and solution. However, the behaviors at solid/liquid interface are very complicated, and the mechanism of CO2RR on those catalyst is not clear. Here, by combining density functional theory and molecular dynamics simulation, this work aims to investgate the CO2RR at M-N-Gra/solution interface to achieve structure and reaction kinetics of this reaction system near the real reaction conditions, especially on the effects of water molecules, species in water and electrode potential, to provide a better understaning of the CO2RR and find efficient CO2RR conditions and catalysts based on M-N-Gra.