File Download

There are no files associated with this item.

  • Find it @ UNIST can give you direct access to the published full text of this article. (UNISTARs only)
Related Researcher

정윤석

Jung, Yoon Seok
Read More

Views & Downloads

Detailed Information

Cited time in webofscience Cited time in scopus
Metadata Downloads

Using Atomic Layer Deposition to Hinder Solvent Decomposition in Lithium Ion Batteries: First-Principles Modeling and Experimental Studies

Author(s)
Leung, KevinQi, YueZavadil, Kevin R.Jung, Yoon SeokDillon, Anne C.Cavanagh, Andrew S.Lee, Se-HeeGeorge, Steven M.
Issued Date
2011-09
DOI
10.1021/ja205119g
URI
https://scholarworks.unist.ac.kr/handle/201301/3716
Fulltext
http://www.scopus.com/inward/record.url?partnerID=HzOxMe3b&scp=80052791129
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.133, no.37, pp.14741 - 14754
Abstract
Passivating lithium ion (Li) battery electrode surfaces to prevent electrolyte decomposition is critical for battery operations. Recent work on conformal atomic layer deposition (ALD) coating of anodes and cathodes has shown significant technological promise. ALD further provides well-characterized model platforms for understanding electrolyte decomposition initiated by electron tunneling through a passivating layer. First-principles calculations reveal two regimes of electron transfer to adsorbed ethylene carbonate molecules (EC, a main component of commercial electrolyte), depending on whether the electrode is alumina coated. On bare Li metal electrode surfaces, EC accepts electrons and decomposes within picoseconds. In contrast, constrained density functional theory calculations in an ultrahigh vacuum setting show that, with the oxide coating, e(-) tunneling to the adsorbed EC falls within the nonadiabatic regime. Here the molecular reorganization energy, computed in the harmonic approximation, plays a key role in slowing down electron transfer. Ab initio molecular dynamics simulations conducted at liquid EC electrode interfaces are consistent with the view that reactions and electron transfer occur right at the interface. Microgravirnetric measurements demonstrate that the ALD coating decreases electrolyte decomposition and corroborates the theoretical predictions.
Publisher
AMER CHEMICAL SOC
ISSN
0002-7863
Keyword
DENSITY-FUNCTIONAL THEORYMOLECULAR-DYNAMICS SIMULATIONSOLID-ELECTROLYTE INTERFACETOTAL-ENERGY CALCULATIONSBINARY REACTION SEQUENCENANOPOROUS-CARBON-FILMSWAVE BASIS-SETETHYLENE CARBONATESURFACE-CHEMISTRYGRAPHITE ANODE

qrcode

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