Strain-induced crystallization and phase separation used for fabricating a tough and stiff slide-ring solid polymer electrolyte

Kei Hashimoto; Toru Shiwaku; Hiroyuki Aoki; Hideaki Yokoyama; Koichi Mayumi; Kohzo Ito

doi:10.1126/sciadv.adi8505

Strain-induced crystallization and phase separation used for fabricating a tough and stiff slide-ring solid polymer electrolyte

Sci Adv. 2023 Nov 24;9(47):eadi8505. doi: 10.1126/sciadv.adi8505. Epub 2023 Nov 24.

Authors

Kei Hashimoto^{1

2

3}, Toru Shiwaku¹, Hiroyuki Aoki^{4

5}, Hideaki Yokoyama¹, Koichi Mayumi^{1

2}, Kohzo Ito¹

Affiliations

¹ Department of Advanced Materials Science, Graduate School of Frontier Sciences, The University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8561, Japan.
² The Institute for Solid State Physics, The University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581, Japan.
³ Department of Chemistry and Biomolecular Science, Faculty of Engineering, Gifu University, 1-1 Yanagido, Gifu 501-1193, Japan.
⁴ Institute of Materials Structure Science, High Energy Accelerator Research Organization, 203-1 Shirakata, Tokai, Naka-gun, Ibaraki 319-1106, Japan.
⁵ Materials and Life Science Division, J-PARC Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Naka-gun, Ibaraki 319-1195, Japan.

Abstract

The demand for mechanically robust polymer-based electrolytes is increasing for applications to wearable devices. Young's modulus and breaking energy are essential parameters for describing the mechanical reliability of electrolytes. The former plays a vital role in suppressing the short circuit during charge-discharge, while the latter indicates crack propagation resistance. However, polymer electrolytes with high Young's moduli are generally brittle. In this study, a tough slide-ring solid polymer electrolyte (SR-SPE) breaking through this trade-off between stiffness and toughness is designed on the basis of strain-induced crystallization (SIC) and phase separation. SIC makes the material highly tough (breaking energy, 80 to 100 megajoules per cubic meter). Phase separation in the polymer enhanced stiffness (Young's modulus, 10 to 70 megapascals). The combined effect of phase separation and SIC made SR-SPE tough and stiff, while these mechanisms do not impair ionic conductivity. This SIC strategy could be combined with other toughening mechanisms to design tough polymer gel materials.