Energetics and Kinetics of Hydrogen Electrosorption on a Graphene-Covered Pt(111) Electrode

Pt(111) surface-membrane interaction 13. Climate action graphene proton permeation 02 engineering and technology 0210 nano-technology 01 natural sciences 7. Clean energy electroadsorption 0104 chemical sciences
DOI: 10.1021/jacsau.2c00648 Publication Date: 2023-01-18T16:46:06Z
ABSTRACT
The Angstrom-scale space between graphene and its substrate provides an attractive playground for scientific exploration and can lead to breakthrough applications. Here, we report the energetics and kinetics of hydrogen electrosorption on a graphene-covered Pt(111) electrode using electrochemical experiments, in situ spectroscopy, and density functional theory calculations. The graphene overlayer influences the hydrogen adsorption on Pt(111) by shielding the ions from the interface and weakening the Pt-H bond energy. Analysis of the proton permeation resistance with controlled graphene defect density proves that the domain boundary defects and point defects are the pathways for proton permeation in the graphene layer, in agreement with density functional theory (DFT) calculations of the lowest energy proton permeation pathways. Although graphene blocks the interaction of anions with the Pt(111) surfaces, anions do adsorb near the defects: the rate constant for hydrogen permeation is sensitively dependent on anion identity and concentration.
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