jp1c03323_si_001.pdf (1.17 MB)
A Universal Approach to Quantify Overpotential-Dependent Selectivity Trends for the Competing Oxygen Evolution and Peroxide Formation Reactions: A Case Study on Graphene Model Electrodes
journal contribution
posted on 2021-05-11, 17:35 authored by Anna Ivanova, Andrew Chesnokov, Dmitry Bocharov, Kai S. ExnerIn this article, we study the competing
oxygen evolution and hydrogen
peroxide (H2O2) formation reactions for periodic
models of graphene with different active-site concentrations by means
of density functional theory (DFT) calculations. Linking the DFT calculations
to ab-initio thermodynamic considerations in conjunction with microkinetic
modeling enables gaining deep insights into the activity and selectivity
trends of graphene-based electrodes as a function of applied bias.
We illustrate that both the coverage of intermediates on the electrode
surface and the applied electrode potential have a significant effect
on the Faradaic efficiency for the electrocatalytic production of
H2O2. The presented approach to study overpotential-dependent
selectivity trends allows deriving design criteria for peroxide formation,
which may serve as a guideline for further studies to realize selective
formation of H2O2 using carbon-based materials.
History
Usage metrics
Categories
Keywords
graphene-based electrodescarbon-based materialselectrode surfacehydrogen peroxideelectrocatalytic productionstudy overpotential-dependent selec...active-site concentrationsUniversal Approachformation reactionsGraphene Model Electrodesmicrokinetic modelingDFT calculationsperoxide formationPeroxide Formation Reactionsdesign criteriaQuantify Overpotential-Dependent Se...oxygen evolutionFaradaic efficiencyselectivity trendsCase StudyH 2 O 2Oxygen Evolution