Electrochemistry from first-principles in the grand canonical ensemble - Publikacja - MOST Wiedzy

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Electrochemistry from first-principles in the grand canonical ensemble

Abstrakt

Progress 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

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Wersja publikacji
Accepted albo Published Version
Licencja
Copyright (2021 AIP Publishing)

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Informacje szczegółowe

Kategoria:
Publikacja w czasopiśmie
Typ:
artykuły w czasopismach
Opublikowano w:
JOURNAL OF CHEMICAL PHYSICS nr 155,
ISSN: 0021-9606
Język:
angielski
Rok wydania:
2021
Opis bibliograficzny:
Bhandari A., Peng C., Dziedzic J., Anton L., Owen J. R., Kramer D., Skylaris C.: Electrochemistry from first-principles in the grand canonical ensemble// JOURNAL OF CHEMICAL PHYSICS -Vol. 155,iss. 2 (2021), s.024114-
DOI:
Cyfrowy identyfikator dokumentu elektronicznego (otwiera się w nowej karcie) 10.1063/5.0056514
Weryfikacja:
Politechnika Gdańska

wyświetlono 85 razy

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