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Sustainable, Dendrite Free Lithium-Metal Electrode Cycling Achieved with Polymer Composite Electrolytes Based on a Poly(Ionic Liquid) Host

Girard, GMA and Wang, X and Yunis, R and MacFarlane, DR and Bhattacharyya, AJ and Forsyth, M and Howlett, PC (2019) Sustainable, Dendrite Free Lithium-Metal Electrode Cycling Achieved with Polymer Composite Electrolytes Based on a Poly(Ionic Liquid) Host. In: Batteries and Supercaps, 2 (3). pp. 229-239.

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Official URL: https://doi.org/10.1002/batt.201800120


Polymer composite solid-state electrolyte materials based on ionic liquids stand out as viable alternatives to flammable liquid electrolytes for solid state lithium-metal batteries. They offer a compromise between favourable mechanical properties and stability against Li-metal, coupled with favourable ion transport. However, insufficient Li+ transport properties for practical battery operation may result from the higher mobility of other ionic species from the ionic liquid (IL). Here, this issue was addressed by confining a highly concentrated IL electrolyte in a poly(ionic liquid) matrix with the addition of 5 wt % of alumina nanoparticles; these superconcentrated IL electrolytes favour Li+ ion transport. The composites are based on a poly(diallyldimethylammonium) bis(trifluoromethanesulfonyl)imide (PDADMA NTf2) matrix, and an electrolyte solution (ES) of high lithium concentration phosphonium IL, trimethyl(isobutyl)phosphonium bis(fluorosulfonyl)imide (P111i4FSI), with 3.8 mol kg−1 (3.8 m) LiFSI. The impact of ES content within the composite on Li+ transference number and electrochemical stability against Li-metal is reported. For the 50 wt % ES and 50 wt % of PDADMA NTf2 composite, up to 0.5 mAh cm−2 of Li-metal plating/stripping for over 20 days at 50 °C is shown. Scanning electron microscopy (SEM) confirmed that no Li dendrite formation was visible at the Li-metal/polymer composite interface. Competitive performance of LiFePO4 electrodes (1.2 mAh cm−2) is also reported.

Item Type: Journal Article
Publication: Batteries and Supercaps
Publisher: Wiley-VCH Verlag
Additional Information: The copyright for this article belongs to the Authors.
Keywords: Alumina; Aluminum oxide; Composite materials; Electrodes; Flammable materials; Ionic liquids; Ions; Iron compounds; Lithium; Lithium batteries; Lithium compounds; Lithium metallography; Plating; Scanning electron microscopy; Solid electrolytes; Solid-State Batteries, Ion transports; Lithium metals; PDADMA; Phosphonium ionic liquid; Polymer composite, Polyelectrolytes
Department/Centre: Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Date Deposited: 28 Oct 2022 05:36
Last Modified: 28 Oct 2022 05:36
URI: https://eprints.iisc.ac.in/id/eprint/77713

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