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

Overview

Journal JACS Au

Publisher American Chemical Society

Specialty Chemistry

Date 2023 Mar 6

PMID 36873699

Authors

Nakkiran Arulmozhi

Selwyn Hanselman

Viorica Tudor

Xiaoting Chen

David van Velden

Gregory F Schneider

Federico Calle-Vallejo

Marc T M Koper

Affiliations

Soon will be listed here.

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.

Citing Articles

Deconvolution of the Voltammetric Features of a Pt(100) Single-Crystal Electrode.

Chen X, Ojha K, Koper M J Phys Chem Lett. 2024; 15(18):4958-4964.

PMID: 38687840 PMC: 11089564. DOI: 10.1021/acs.jpclett.4c01056.

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