Atomistic mechanisms of hard carbon formation from polyvinylidene chloride.
- 1Inorganic Chemistry Laboratory, Department of Chemistry, University of Oxford Oxford UK [email protected].
Abstract
Hard carbons are a class of disordered materials with widespread application in energy storage. Despite decades of research, their atomistic formation mechanisms have remained elusive, due to the difficulty of both in situ experimental characterization and first-principles simulations. Here, we describe the formation mechanism of hard carbon from the thermal decomposition of polyvinylidene chloride (PVDC), using first-principles-quality simulations with a bespoke machine-learned interatomic potential model. Our results indicate a two-stage process, consisting of (i) radical-mediated dehydrochlorination, which generates reactive unsaturated carbon sites, and (ii) progressive carbon-carbon cross-linking followed by thermally activated rearrangement into an extended sp2-bonded network. We provide an atomistic account of non-hexagonal ring motifs emerging during pyrolysis, supporting the established theory that these motifs induce the intrinsic curvature that frustrates graphitic ordering in hard carbons.
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BibTeX
@article{wu2026atomistic,
title = {{Atomistic mechanisms of hard carbon formation from polyvinylidene chloride.}},
author = {Litong Wu and Zitong Wu and Zakariya El-Machachi and Volker L Deringer},
journal = {Chemical science},
year = {2026},
month = oct,
doi = {10.1039/d6sc05974k},
url = {https://europepmc.org/article/MED/42953584},
note = {CC BY},
}
RIS
TY - JOUR
TI - Atomistic mechanisms of hard carbon formation from polyvinylidene chloride.
AU - Litong Wu
AU - Zitong Wu
AU - Zakariya El-Machachi
AU - Volker L Deringer
PY - 2026
DA - 2026/10/08
JO - Chemical science
DO - 10.1039/d6sc05974k
UR - https://europepmc.org/article/MED/42953584
AB - Hard carbons are a class of disordered materials with widespread application in energy storage. Despite decades of research, their atomistic formation mechanisms have remained elusive, due to the difficulty of both in situ experimental characterization and first-principles simulations. Here, we describe the formation mechanism of hard carbon from the thermal decomposition of polyvinylidene chloride (PVDC), using first-principles-quality simulations with a bespoke machine-learned interatomic potential model. Our results indicate a two-stage process, consisting of (i) radical-mediated dehydrochlorination, which generates reactive unsaturated carbon sites, and (ii) progressive carbon-carbon cross-linking followed by thermally activated rearrangement into an extended sp2-bonded network. We provide an atomistic account of non-hexagonal ring motifs emerging during pyrolysis, supporting the established theory that these motifs induce the intrinsic curvature that frustrates graphitic ordering in hard carbons.
SN - 2041-6520
SN - 2041-6539
ER -