Synergistically regulating the separator pore structure and surface property toward dendrite-free and high-performance aqueous zinc-ion batteries.

As an emerging electrochemical device, aqueous zinc-ion batteries (ZIBs) present promising potential in safe and large-scale energy storage. However, the large pores of commercial glass fiber (GF) separators result in uneven Zn2+ ion flux, leading to severe dendrite growth issues of Zn metal anodes. Herein, we integrated a multifunctional layer on the GF separator that can synergistically regulate the pore feature and surface property of commercial GF separators. Such modification layer, composed of nanocellulose and SiO2 nanoparticles, exhibited uniform nanoporous structure and abundant negatively charged polar functional groups. These features allow regulating the distribution of Zn2+ ions at the separator-anode interface, facilitating stable and uniform Zn nucleation and growth. Moreover, the electrostatic interaction between the negatively charged functional groups and Zn2+ ions enhanced the Zn2+ ion transport kinetics, preventing the Zn dendrites formation and adverse reactions. Consequently, the modified electrolyte-filled GF separator showed an increased Zn2+ ion transference number of 0.65. The symmetric Zn//Zn batteries utilizing such a separator achieved an impressive cycling life of 500 h at a high current density/capacity of 10 mA cm-2/4 mAh cm-2, nearly nine times longer than the battery using the unmodified GF separator (<55 h). The superior electrochemical performance was verified in both Zn//AC and Zn//LiMn2O4 full battery evaluations. This work presents a novel synergistic modification strategy for developing advanced separators for aqueous ZIBs.

Rational Design of Zincophilic Ag/Permselective PEDOT:PSS Heterogeneous Interfaces for High-Rate Zinc Electrodeposition.

Designing artificial interface is a promising strategy to protect Zn metal anode but achieving long Zn plating/stripping lifespans and efficient nucleation/deposition kinetics, particularly at high current densities, remains a challenge. In this study, a permselective zincophilic heterogeneous interface consisting of metallic Ag layer and poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is designed via a simple chemical displacement and drop casting process. The artificial interface plays a multifunctional role in inhibiting dendrite growth/side reactions by reducing the nucleation barrier through a large number of Zn nucleation sites offered by the bottom Ag layer, homogenizing electrical field/Zn2+ flux and shielding SO4 2- migration via the compact, conducting, and Zn2+ -permselective PEDOT:PSS supporting layer. Moreover, the heterogeneous interface demonstrates enhanced structural integrity owing to the binder effect of PEDOT:PSS. As a result, the modified Zn anode demonstrates a cyclic lifespan of 200 h and a reduced voltage hysteresis of ≈150 mV at 20 mA cm-2 /5 mAh cm-2 , far surpassing its counterparts. Moreover, the protected Zn anode allows the LiMn2 O4 -based full cells with remarkable rate and cycling performance. These findings provide new insight into the design of an efficient artificial interface for highly reversible and high-rate Zn electrodeposition.