How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction.
Xiaoting ChenLaura P Granda-MarulandaIan T McCrumMarc T M KoperPublished in: Nature communications (2022)
Development of reversible and stable catalysts for the electrochemical reduction of CO 2 is of great interest. Here, we elucidate the atomistic details of how a palladium electrocatalyst inhibits CO poisoning during both formic acid oxidation to carbon dioxide and carbon dioxide reduction to formic acid. We compare results obtained with a platinum single-crystal electrode modified with and without a single monolayer of palladium. We combine (high-scan-rate) cyclic voltammetry with density functional theory to explain the absence of CO poisoning on the palladium-modified electrode. We show how the high formate coverage on the palladium-modified electrode protects the surface from poisoning during formic acid oxidation, and how the adsorption of CO precursor dictates the delayed poisoning during CO 2 reduction. The nature of the hydrogen adsorbed on the palladium-modified electrode is considerably different from platinum, supporting a model to explain the reversibility of this reaction. Our results help in designing catalysts for which CO poisoning needs to be avoided.
Keyphrases
- carbon dioxide
- reduced graphene oxide
- density functional theory
- gold nanoparticles
- hydrogen peroxide
- carbon nanotubes
- solid state
- metal organic framework
- electron transfer
- highly efficient
- molecular dynamics
- computed tomography
- healthcare
- molecular dynamics simulations
- nitric oxide
- high resolution
- magnetic resonance