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Nanocellulose-Induced Surface-Lock Engineering: Curbing the Dissolution of MnO2 for High-Performance Zn-MnO2 Flexible Electrodes
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DOI：10.1002/cey2.70097.png)
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Abstract
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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 degrees) 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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