Density functional theory screening of gas-treatment strategies for stabilization of high energy-density lithium metal anodes

Koch, Stephan L, Morgan, Benjamin J, Passerini, Stefano and Teobaldi, Gilberto ORCID: 0000-0001-6068-6786 (2015) Density functional theory screening of gas-treatment strategies for stabilization of high energy-density lithium metal anodes. JOURNAL OF POWER SOURCES, 296. pp. 150-161.

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Official URL: http://dx.doi.org/10.1016/j.jpowsour.2015.07.027

Abstract

To explore the potential of molecular gas treatment of freshly cut lithium foils in non-electrolyte based passivation of high energy-density Li anodes, density functional theory (DFT) has been used to study the decomposition of molecular gases on metallic lithium surfaces. By combining DFT geometry optimization and Molecular Dynamics, the effects of atmospheric (N2, O2, CO2) and hazardous (F2, SO2) gas decomposition on Li(bcc) (100), (110), and (111) surfaces on relative surface energies, work functions, and emerging electronic and elastic properties are investigated. The simulations suggest that exposure to different molecular gases can be used to induce and control reconstructions of the metal Li surface and substantial changes (up to over 1 eV) in the work function of the passivated system. Contrary to the other considered gases, which form metallic adlayers, SO2 treatment emerges as the most effective in creating an insulating passivation layer for dosages <= 1 mono-layer. The substantial Li->adsorbate charge transfer and adlayer relaxation produce marked elastic stiffening of the interface, with the smallest change shown by nitrogen-treated adlayers.

Item Type:	Article
Uncontrolled Keywords:	Density functional theory, Lithium metal gas treatment, Surface reconstruction, Artificial solid electrolyte interphase, Work function, Elasticity
Subjects:	?? QC ?? ?? QD ??
Depositing User:	Symplectic Admin
Date Deposited:	04 Aug 2015 09:55
Last Modified:	16 Dec 2022 15:58
DOI:	10.1016/j.jpowsour.2015.07.027
Open Access URL:	http://www.sciencedirect.com/science/article/pii/S...
Related URLs:	Author Publisher
URI:	https://livrepository.liverpool.ac.uk/id/eprint/2018723