Breaking Water at Graphene Defects
Abstract
Water dissociation at solid surfaces underpins processes ranging from corrosion and catalysis to electrochemistry and photovoltaics. Defects often serve as reactive sites for dissociation, yet how solvation influences water dissociation at such sites remains poorly understood. Here, we use state-of-the-art machine-learned interatomic potentials to explore water dissociation at defective graphene-water interfaces. We show that solvation qualitatively changes the reaction mechanism at a graphene single vacancy (SV), opening pathways that are absent for an isolated water molecule. Whereas the gas-phase process proceeds via a single concerted channel, the solvated SV splits water through two competing pathways: a basic route forming SV-H and OH-(aq), and an acidic route forming SV-OH and H3O+(aq). These lower-barrier pathways produce distinct chemisorbed intermediates that enhance graphene-water adsorption. Accordingly, even a simple carbon vacancy gives rise to unexpectedly rich interfacial chemistry, coupling surface chemistry to interfacial charge and wettability, with implications for carbon functionalization and nanofluidic transport.
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BibTeX
@misc{brookes2026breaking,
title = {{Breaking Water at Graphene Defects}},
author = {Samuel G. H. Brookes and IniOluwa C. Popoola and Fabian Berger and Kara D. Fong and Angelos Michaelides and Christoph Schran},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.11602},
eprint = {2609.11602},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.11602},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Breaking Water at Graphene Defects
AU - Samuel G. H. Brookes
AU - IniOluwa C. Popoola
AU - Fabian Berger
AU - Kara D. Fong
AU - Angelos Michaelides
AU - Christoph Schran
PY - 2026
DA - 2026/09/10
PB - arXiv
DO - 10.48550/arxiv.2609.11602
UR - https://arxiv.org/abs/2609.11602
AB - Water dissociation at solid surfaces underpins processes ranging from corrosion and catalysis to electrochemistry and photovoltaics. Defects often serve as reactive sites for dissociation, yet how solvation influences water dissociation at such sites remains poorly understood. Here, we use state-of-the-art machine-learned interatomic potentials to explore water dissociation at defective graphene-water interfaces. We show that solvation qualitatively changes the reaction mechanism at a graphene single vacancy (SV), opening pathways that are absent for an isolated water molecule. Whereas the gas-phase process proceeds via a single concerted channel, the solvated SV splits water through two competing pathways: a basic route forming SV-H and OH-(aq), and an acidic route forming SV-OH and H3O+(aq). These lower-barrier pathways produce distinct chemisorbed intermediates that enhance graphene-water adsorption. Accordingly, even a simple carbon vacancy gives rise to unexpectedly rich interfacial chemistry, coupling surface chemistry to interfacial charge and wettability, with implications for carbon functionalization and nanofluidic transport.
ER -