DC FieldValueLanguage
dc.contributor.authorBhandari, Arihant-
dc.contributor.authorPeng, Chao-
dc.contributor.authorDziedzic, Jacek-
dc.contributor.authorAnton, Lucian-
dc.contributor.authorOwen, John R.-
dc.contributor.authorKramer, Denis-
dc.contributor.authorSkylaris, Chris-Kriton-
dc.date.accessioned2022-05-13T12:58:25Z-
dc.date.available2022-05-13T12:58:25Z-
dc.date.issued2021-07-12-
dc.identifier.issn0021-9606-
dc.descriptionFunding Information: This work was carried out with funding from the Faraday Institution (faraday.ac.uk; EP/S003053/1), Grant No. FIRG003. The majority of computations presented in this work were performed on the Iridis 5 supercomputer of the University of Southampton and the Michael supercomputer of the Faraday Institution. We acknowledge the United Kingdom Materials and Molecular Modeling Hub for computational resources, partially funded by the EPSRC (Grant Nos. EP/P020194/1 and EP/T022213/1). Publisher Copyright: {\textcopyright} 2021 Author(s). Copyright: Copyright 2021 Elsevier B.V., All rights reserved.-
dc.description.abstractProgress in electrochemical technologies, such as automotive batteries, supercapacitors, and fuel cells, depends greatly on developing improved charged interfaces between electrodes and electrolytes. The rational development of such interfaces can benefit from the atomistic understanding of the materials involved by first-principles quantum mechanical simulations with Density Functional Theory (DFT). However, such simulations are typically performed on the electrode surface in the absence of its electrolyte environment and at constant charge. We have developed a new hybrid computational method combining DFT and the Poisson-Boltzmann equation (P-BE) capable of simulating experimental electrochemistry under potential control in the presence of a solvent and an electrolyte. The charged electrode is represented quantum-mechanically via linear-scaling DFT, which can model nanoscale systems with thousands of atoms and is neutralized by a counter electrolyte charge via the solution of a modified P-BE. Our approach works with the total free energy of the combined multiscale system in a grand canonical ensemble of electrons subject to a constant electrochemical potential. It is calibrated with respect to the reduction potential of common reference electrodes, such as the standard hydrogen electrode and the Li metal electrode, which is used as a reference electrode in Li-ion batteries. Our new method can be used to predict electrochemical properties under constant potential, and we demonstrate this in exemplar simulations of the differential capacitance of few-layer graphene electrodes and the charging of a graphene electrode coupled to a Li metal electrode at different voltages.-
dc.description.sponsorshipComputational Material Design-
dc.language.isoeng-
dc.publisherAmerican Institute of Physics-
dc.relation.ispartofThe journal of chemical physics : JCP-
dc.titleElectrochemistry from first-principles in the grand canonical ensemble-
dc.typeArticle-
dc.identifier.doi10.1063/5.0056514-
dcterms.bibliographicCitation.volume155-
dcterms.bibliographicCitation.issue2-
dcterms.bibliographicCitation.originalpublisherplaceMelville, NY-
local.submission.typeonly-metadata-
dc.type.articleScientific Article-
hsu.peerReviewed✅-
item.grantfulltextnone-
item.languageiso639-1en-
item.fulltext_sNo Fulltext-
item.openairetypeArticle-
item.fulltextNo Fulltext-
crisitem.author.deptComputational Material Design-
crisitem.author.parentorgFakultät für Maschinenbau und Bauingenieurwesen-
Appears in Collections:3 - Publication references (without fulltext)
Show simple item record

CORE Recommender

SCOPUSTM   
Citations

12
checked on Apr 6, 2024

Google ScholarTM

Check

Altmetric

Altmetric

User Tools
Login to see more information

Items in openHSU are protected by copyright, with all rights reserved, unless otherwise indicated.