Abstract

Dendrite formation and water-induced side reactions are critical factors in limiting the reversibility of Zn metal

anodes in aqueous Zn-ion batteries (AZIBs). Herein, we investigate how three different carbon materials—carbon

black (CB), carbon nanotubes (CNT), and reduced graphene oxide (rGO)—influence microstructure (e.g. polymer

mobility and porosity) and Zn-adsorption affinity of polyvinylidene fluoride (PVDF)/carbon porous passivation

layers formed via a nonsolvent-induced phase separation method through combined electrochemical analyses

and first-principles density functional theory calculations. We found that PVDF/CNT exhibited the lowest

PVDF–carbon interaction energy yet the highest Zn adsorption affinity compared to PVDF/CB and PVDF/rGO.

This balanced interaction promotes the formation of relatively uniform porosity, enabling stable Zn deposition

and reversible Zn plating/stripping behavior. The optimized PVDF/CNT-coated Zn anode achieves over 2400 h of

cycling at 1 mA cm-2 in symmetric cells and significantly improves capacity retention in MnO2 full cells

compared with pristine Zn. Furthermore, 3 × 3 cm2 pouch cells with PVDF/CNT-coated Zn anodes retained

73.5% of their initial capacity after 100 cycles. These results highlight an interfacial engineering strategy that

leverages carbon–polymer interactions to enable durable AZIB technologies.

링크: https://www.sciencedirect.com/science/article/pii/S1385894726062790