Reaction mechanism and kinetics for CO₂ reduction on nickel single atom catalysts from quantum mechanics.

ABSTRACT: Experiments have shown that graphene-supported Ni-single atom catalysts (Ni-SACs) provide a promising strategy for the electrochemical reduction of CO₂ to CO, but the nature of the Ni sites (Ni-N₂C₂, Ni-N₃C₁, Ni-N₄) in Ni-SACs has not been determined experimentally. Here, we apply the recently developed grand canonical potential kinetics (GCP-K) formulation of quantum mechanics to predict the kinetics as a function of applied potential (U) to determine faradic efficiency, turn over frequency, and Tafel slope for CO and H₂ production for all three sites. We predict an onset potential (at 10 mA cm^-2) U_onset = -0.84 V (vs. RHE) for Ni-N₂C₂ site and U_onset = -0.92

SUBMITTER: Hossain MD 

PROVIDER: S-EPMC7205999 | biostudies-literature | 2020 May

REPOSITORIES: biostudies-literature