Lithium-Ion Battery Solid Electrolytes Based on Poly(vinylidene Fluoride)-Metal Thiocyanate Ionic Liquid Blends

João P Serra; Arkaitz Fidalgo-Marijuan; João C Barbosa; Daniela M Correia; Renato Gonçalves; José M Porro; Senentxu Lanceros-Mendez; Carlos M Costa

doi:10.1021/acsapm.2c00789

Lithium-Ion Battery Solid Electrolytes Based on Poly(vinylidene Fluoride)-Metal Thiocyanate Ionic Liquid Blends

ACS Appl Polym Mater. 2022 Aug 12;4(8):5909-5919. doi: 10.1021/acsapm.2c00789. Epub 2022 Jul 13.

Authors

João P Serra^{1

2}, Arkaitz Fidalgo-Marijuan^{3

4}, João C Barbosa^{1

2

5}, Daniela M Correia^{1

5}, Renato Gonçalves⁶, José M Porro^{3

7}, Senentxu Lanceros-Mendez^{3

7}, Carlos M Costa^{1

2

8}

Affiliations

¹ Physics Centre of Minho and Porto Universities (CF-UM-UP), University of Minho, Braga 4710-057, Portugal.
² Laboratory of Physics for Materials and Emergent Technologies, LapMET, University of Minho, Braga 4710-057, Portugal.
³ BCMaterials, Basque Center for Materials, Applications and Nanostructures, UPV/EHU Science Park, 48940 Leioa, Spain.
⁴ Department of Organic and Inorganic Chemistry, University of the Basque Country (UPV/EHU), 48940 Leioa, Spain.
⁵ Centre of Chemistry, University of Trás-os-Montes e Alto Douro, 5000-801 Vila Real, Portugal.
⁶ Centre of Chemistry, University of Minho, 4710-057 Braga, Portugal.
⁷ Ikerbasque, Basque Foundation for Science, 48009 Bilbao, Spain.
⁸ Institute of Science and Innovation for Bio-Sustainability (IB-S), University of Minho, 4710-057 Braga, Portugal.

Abstract

Solid polymer electrolytes (SPEs) are required to improve battery safety through the elimination of the liquid electrolyte solution in current batteries. This work is focused on the development of a hybrid SPE based on poly(vinylidene fluoride), PVDF, and 1-butyl-3-methylimidazolium cobalt(II) isothiocyanate, [BMIM]₂[(SCN)₄Co] magnetic ionic liquid (MIL), and its battery cycling behavior at room temperature. The addition of MIL in filler contents up to 40 wt % to the PVDF matrix does not influence the compact morphology of the samples obtained by solvent casting. The polar β-phase of PVDF increases with increasing MIL content, whereas the degree of crystallinity, thermal degradation temperature, and mechanical properties of the MIL/PVDF blends decrease with increasing MIL content. The ionic conductivity of the MIL/PVDF blends increases both with temperature and MIL content, showing the highest ionic conductivity of 7 × 10^-4 mS cm^-1 at room temperature for the MIL/PVDF blend with 40 wt % of MIL. The cathodic half-cells prepared with this blend as SPE show good reversibility and excellent cycling behavior at different C-rates, with a discharge capacity of 80 mAh g^-1 at a C/10-rate with a Coulombic efficiency of 99%. The developed magnetic SPE, with excellent performance at room temperature, shows potential for the implementation of sustainable lithium-ion batteries, which can be further tuned by the application of an external magnetic field.