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
AUTHORS (8)
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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