ISSN print edition: 0366-6352 ISSN electronic edition: 1336-9075 Registr. No.: MK SR 9/7 Published monthly

Design of robust hydrogel electrolytes via cellulose nanofiber-induced hydrogen bonding for enhanced hydroxide transport

Hengyuan Dong, Fanting Wu, Jinshan Zhang, Guotao Zhang, Qiang Wang, Weiliang Liu, Hao Yu, Cong Li, Xiaoxia Cai, and Yanlin Sun

School of Materials Science & Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan, China

E-mail: 19861406603@163.com

Received: 30 September 2025  Accepted: 20 April 2026

Abstract:

The advancement of flexible zinc-air batteries is constrained by the performance trade-off in their core component—alkaline hydrogel electrolytes—which often struggle to balance mechanical robustness with high ionic conductivity. To address this challenge, this study proposes a strategy of constructing multiple hydrogen-bonding networks induced by cellulose nanofibers (CNF) to design gel electrolytes that simultaneously exhibit superior mechanical durability and excellent hydroxide ion transport. Specifically, a polyvinyl alcohol (PVA)/CNF-based alkaline PVA/N-PAM/CNF hydrogel with a hydrogen-bond-rich architecture was successfully synthesized through in-situ polymerization of acrylamide (AM) within a PVA/CNF matrix, followed by a freeze-thaw cycling process. This uniquely engineered network endows the hydrogel with an exceptional ionic conductivity of 353.36 mS cm⁻¹, while also delivering outstanding mechanical properties, including a tensile strength of 690.55 kPa, an elongation at break of 385.17%, and a toughness of 1.67 MJ m⁻³. Furthermore, the incorporation of CNF significantly enhances the electrolyte’s alkali absorption capacity and water retention capability. When deployed in a flexible zinc-air battery, this PVA/N-PAM/CNF hydrogel electrolyte enables remarkable performance: a cycle life of 236 cycles, an energy density of 50.04 mW cm⁻², and an extended discharge duration of 938 min.

Keywords: Hydrogel electrolyte; Polyvinyl alcohol; Polyacrylamide; Cellulose nanofiber; Hydrogen bonding; Flexible Zn-air battery

Full paper is available at www.springerlink.com.

DOI: 10.1007/s11696-026-04959-3

Chemical Papers 80 (8) 9401–9413 (2026)