CO2 Crossover to the Li Anode and Its Implications on the Solid Electrolyte Interphase Composition in a Rechargeable Li-CO2 Battery

Bharti, A and Deb, D and Achutharao, G and Bhattacharyya, AJ (2024) CO2 Crossover to the Li Anode and Its Implications on the Solid Electrolyte Interphase Composition in a Rechargeable Li-CO2 Battery. In: Journal of Physical Chemistry C .

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Abstract

A major fundamental challenge in a Li-CO2 battery, which has not received due attention in comparison to the intricacies of CO2 redox, is the CO2 gas crossover toward the Li anode. The CO2 crossover during battery operation changes the Li chemical state and the composition of the proximate solid electrolyte interphase (SEI). Systematic ex situ Raman spectroscopy and X-ray diffraction investigations confirm continuous active Li metal depletion with successive cycles due to CO2 (or CO2/O2) crossover. Irrespective of the gas, our studies convincingly reveal active Li metal conversion to majorly LiOH and Li2CO3, with LiOH being the dominant phase at higher cycle numbers. Depth profile X-ray photoelectron spectroscopy reveals additional SEI components, viz., Li2O, Li2S, LiF, and CF3, which exhibit a depth-dependent spatial distribution along with Li2CO3 and LiOH. Analytical chemical investigations based on metalation reactions quantitatively reveal irreversible loss of active Li metal with successive cycling. © 2024 American Chemical Society.

Item Type:	Journal Article
Publication:	Journal of Physical Chemistry C
Publisher:	American Chemical Society
Additional Information:	The copyright for this article belongs to American Chemical Society.
Keywords:	Anodes; Carbon dioxide; Lithium; Solid electrolytes; X ray photoelectron spectroscopy, Battery operation; Chemical state; Dominant phasis; Ex situ; High cycle; Li metal; Li-anodes; Situ Raman spectroscopy; Solid electrolyte interphase; X-ray diffraction investigations, Lithium compounds
Department/Centre:	Division of Chemical Sciences > Solid State & Structural Chemistry Unit Division of Interdisciplinary Sciences > Interdisciplinary Centre for Energy Research
Date Deposited:	18 Dec 2024 09:52
Last Modified:	18 Dec 2024 09:52
URI:	http://eprints.iisc.ac.in/id/eprint/85870

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