Bio-derived polymer-based electrolytes for Lithium-metal batteries

Raj, Ashish
(2024)

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Authors
  • Raj, AshishUCLouvain
    author
Supervisors
Gohy, Jean-François
Abstract
Solid-state batteries are expected to upgrade the lithium battery (LB) technology with their safety, higher energy density and superior characteristics over conventional liquid electrolyte-based LIB. Polymers based on polyethylene oxide (PEO), polycarbonate etc. are front runners toward this goal in realization of solid polymer electrolytes. However, most of these polymers have relatively less environmental benignity. Counting on that, bio-derived polymers synthesized through non-toxic routes excite many researchers, including us, leading to the core motivation of this thesis. We synthesized a series of polymers via facile chemistry starting from solvent-free viscous monomer carbonated soybean oil (CSBO) to poly(hydroxyurethanes) (PHU) network and their analogues. The work carried out in this thesis is classified into three categories: a) Non-opened cyclic carbonate (CC), b) ring-opened CC, PHU and c) composite polymer electrolyte. Novel non-isocyanate and catalyst-free methods were exploited for the synthesis of these PHU networks via polyaddition includind blending, plasticization and composites, respectively. We were able to achieve ionic conductivity in the range of 10-6 to 10-3 S cm-1 for various formulations with an electrochemical stability window as high as ESW > 4.5 V versus Li/Li+. Further, lithium metal battery prototypes fabricated with Lithium ferrophosphate (LiFePO4/LFP) were subjected to coin cell testing for potential limited galvanostatic charge-discharge over several cycles and current densities. The fundamental understanding of the decomposition of an electrolyte subjected to its functionalities has also been one of the key objectives of this work. The thesis covers various states of solvent-free CSBO-derived electrolytes from viscous, gel-like networks to free-standing solid membranes with and without separators targeting attempts to inspire more efforts in bio-derived battery materials with high performance.
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Citations

Raj, A. (2024). Bio-derived polymer-based electrolytes for Lithium-metal batteries. https://hdl.handle.net/2078.5/243026