Tuning Zn2+ coordination tunnel by hierarchical gel electrolyte for dendrite-free zinc anode.

Aqueous zinc-ion batteries (ZIBs) are perceived as one of the most upcoming grid-scale storage systems. However, the issues of electrode dissolution, dendrite formation, and corrosion in traditional liquid electrolytes have plagued its progress. In this work, Zn dendrite growth and side reactions are effectively suppressed by a highly-confined tannic acid (TA) modified sodium alginate (SA) composite gel electrolyte (TA-SA). The ion-confinement effect is enhanced by divalent zinc ions coordinated with carboxyl groups and chelated with phenolic hydroxyl groups, thus guiding and regulating Zn deposition to achieve steady zinc plating/stripping behavior. As a consequence, the Zn/TA-SA/NH4V4O10 full cells deliver a high specific capacity of 238.6 mAh g-1 and maintain 94.51% over 900 cycles at 2 A g-1. Notably, after resting over 5 d, the capacity can be stabilized with a capacity retention of 97.25% after 200 cycles at 2 A g-1. This highly-confined and hydrogen bond-strengthened gel electrolyte may provide an effective strategy for the future development of quasi-solid-state metal batteries.

A smelting-rolling strategy for ZnIn bulk phase alloy anodes.

Reversibility and stability are considered as the key indicators for Zn metal anodes in aqueous Zn-ion batteries, yet they are severely hindered by uncontrolled Zn stripping/plating and side reactions. Herein, we fabricate a bulk phase ZnIn alloy anode containing trace indium by a typical smelting-rolling process. A uniformly dispersed bulk phase of the whole Zn anode is constructed rather than only a protective layer on the surface. The Zn deposition can be regarded as instantaneous nucleation due to the adsorption of the evenly dispersed indium, and formation of the exclusion zone for further nucleation can be prevented at the same time. Owing to the bulk phase structure of ZnIn alloy, the indium not only plays a crucial role in Zn deposition, but also improves the Zn stripping. Consequently, the as-designed ZnIn alloy anode can sustain stable Zn stripping/plating for over 2500 h at 4.4 mA cm-2 with nearly 6 times smaller voltage hysteresis than that of pure Zn. Moreover, it enables a substantially stable ZnIn//NH4V4O10 battery with 96.44% capacity retention after 1000 cycles at 5 A g-1. This method of regulating the Zn nucleation by preparing a Zn-based alloy provides a potential solution to the critical problem of Zn dendrite growth and by-product generation fundamentally.