Cross-Linking of Sugar-Derived Polyethers and Boronic Acids for Renewable, Self-Healing, and Single-Ion Conducting Organogel Polymer Electrolytes

Emma L Daniels; James R Runge; Matthew Oshinowo; Hannah S Leese; Antoine Buchard

doi:10.1021/acsaem.2c03937

Cross-Linking of Sugar-Derived Polyethers and Boronic Acids for Renewable, Self-Healing, and Single-Ion Conducting Organogel Polymer Electrolytes

ACS Appl Energy Mater. 2023 Feb 22;6(5):2924-2935. doi: 10.1021/acsaem.2c03937. eCollection 2023 Mar 13.

Authors

Emma L Daniels^{1

2

3}, James R Runge^{1

2}, Matthew Oshinowo^{1

2}, Hannah S Leese^{1

3}, Antoine Buchard^{1

2}

Affiliations

¹ University of Bath Institute for Sustainability, Claverton Down, Bath BA2 7AY, U.K.
² Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, U.K.
³ Materials for Health Lab, Department of Chemical Engineering, University of Bath, Claverton Down, Bath BA2 7AY, U.K.

Abstract

This report describes the synthesis and characterization of organogels by reaction of a diol-containing polyether, derived from the sugar d-xylose, with 1,4-phenylenediboronic acid (PDBA). The cross-linked materials were analyzed by infrared spectroscopy (FT-IR), thermal gravimetric analysis (TGA), scanning electron microscopy (FE-SEM), and rheology. The rheological material properties could be tuned: gel or viscoelastic behavior depended on the concentration of polymer, and mechanical stiffness increased with the amount of PDBA cross-linker. Organogels demonstrated self-healing capabilities and recovered their storage and loss moduli instantaneously after application and subsequent strain release. Lithiated organogels were synthesized through incorporation of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) into the cross-linked matrix. These lithium-borate polymer gels showed a high ionic conductivity value of up to 3.71 × 10^-3 S cm^-1 at 25 °C, high lithium transference numbers (t ₊ = 0.88-0.92), and electrochemical stability (4.51 V). The gels were compatible with lithium-metal electrodes, showing stable polarization profiles in plating/stripping tests. This system provides a promising platform for the production of self-healing gel polymer electrolytes (GPEs) derived from renewable feedstocks for battery applications.