Nanocellulose-Induced “Surface-Lock” Engineering: Curbing the Dissolution of MnO₂ for High-Performance Zn–MnO₂ Flexible Electrodes

Abstract

Carbon-based substrates in Zn–MnO₂ flexible batteries have issues of low adhesion to MnO₂, impacting cycle stability and capacity performance. A triple-synergistic strategy integrating C–O–Mn covalent bonding, wettability optimization, and hierarchical mesoporous engineering via cellulose nanofibers/carbon nanotube (CNF/CNT)-modified carbon cloth (CC) was proposed. This design achieves a “surface-locking” effect between the substrate and electrode materials, which was proven through theory and experiments. Density functional theory (DFT) simulations validate the “surface-locking” mechanism, where oxygen functionalities on CNF can form robust CO–Mn bonds with MnO₂, inducing an increase in MnO₂ adsorption energy from −0.21 eV (pristine CC) to −1.36 eV, effectively suppressing Mn dissolution. Optimal wettability (contact angle: 97°) reduced Zn²⁺ desolvation and water-induced side reactions. Hierarchical pore structures accelerated Zn²⁺ diffusion. The optimized CC@CNF₁/CNT₂–MnO₂ cathode achieves 92% capacity retention after 2000 cycles at 1 A/g. This study highlights a surface engineering strategy that effectively addresses the individual challenges associated with interfacial adhesion, reaction kinetics, and ion transport. This strategy offers fundamental insights into electrode interface modification for the development of next-generation flexible energy storage systems.

Keywords

cellulose nanofibers / flexible zinc batteries / interface engineering

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