Regulating the Zn deposition orientation is an efficient way to suppress Zn dendrites and stabilize Zn anodes in aqueous Zn ion batteries (ZIBs). Few studies have been conducted to control Zn(002) deposition by altering the Zn2+ solvation structure with a cosolvent. Herein, the bifunctional high-polarity cosolvent hexamethylphosphoramide (HMPA) is proposed in an aqueous electrolyte. It not only suppresses the H2 evolution reaction via the reshaped Zn2+ solvation structure with decreased H2O activity but also induces Zn(002) deposition with a hexagonal-close-packed morphology due to the strong absorption ability of HMPA to Zn(002). With the optimized electrolyte, Zn dendrites and the HER are suppressed and an ultralong cycle life of 1500 cycles with 99.6% Coulombic efficiency is achieved in Zn||Cu cells. Zn||NH4V5O10 and Zn||polyaniline full cells exhibit improved cycling performances compared to that of the bare electrolyte. Our finding provides a feasible and promising way to stabilize Zn anodes and promote the commercial application of ZIBs. 

Regulating Zn(002) Deposition toward Long Cycle Life for Zn Metal Batteries

Advanced aqueous batteries are promising for next generation flexible and wearable devices owing to the high safety, yet still requiring better cycling stability and high specific capacity in wide temperature range. Herein, a polymeric acid hydrogel electrolyte (PAGE) with 3 M Zn(ClO4)2 was fabricated for high performance Zn/polyaniline (PANI) batteries. The -SO3-H+ function group in PAGE can endow the Zn/PANI battery with following merits: firstly, accelerating the redox reaction kinetics for PANI by constant proton generation; secondly, increasing the specific capacity by boosting the reaction sites between ions and PANI functional groups; thirdly, suppressing the side reaction and dendrites by inducing the (002) crystal plane formation. In addition, the anti-freezing performance for the hydrogel is also optimized by the salt and hydrogel, with a high ionic conductivity of 14.2 mS cm-1 at -35oC. As a consequence, even at -35oC, the Zn/Zn symmetrical battery can keep stable for more than 1,500 h under 2 mA cm-2, and the Zn/PANI battery can provide ultra-high stable specific capacity of 79.6 mA h g-1 for more than 70,000 cycles at 15 A g-1. This proton-supplying strategy by polymeric acid hydrogel may further propel the development of high performance aqueous batteries.

Proton-reservoir hydrogel electrolyte for long-term cycling Zn/PANI batteries in wide temperature range.

In situ formation of a stable interphase layer on zinc surface is an effective solution to suppress dendrite growth. However, the fast transport of bivalent Zn-ions within the solid interlayer remains very challenging. Herein, we engineer the SEI components and enable superior kinetics of Zn metal batteries under harsh conditions through regulating the sequence of interfacial chemical reaction. With the differences in chemical reactivity of trimethyl phosphate co-solvent and trifluoromethanesulfonate anions in the Zn2+-solvation shell, Zn3(PO4)2 and ZnF2 are successively generated on Zn metal surface to form a gradient ZnF2-Zn3(PO4)2 interphase. Mechanistic studies reveal the outer ZnF2 facilitates Zn2+ desolvation and inner Zn3(PO4)2 serves as channels for fast Zn2+ transport, contributing to long-term cycling at subzero temperatures. Impressively, the gradient SEI enables a high lifespan over 7000 hours in Zn symmetric cell and a capacity retention of 86.1% after 12000 cycles in Zn-KVOH full cell at -50 °C. 

Regulating interfacial reaction through electrolyte chemistry enables gradient interphase for low-temperature zinc metal batteries.

2-methyl imidazole electrolyte additive enabling ultra-stable Zn anode

Rechargeable aqueous zinc‐ion batteries (AZBs), with their high theoretical capacity, low cost, safety, and environmental friendliness, have risen as a promising candidate for next‐generation energy storage. Despite the fruitful progress in cathode material research, the electrochemical performance of the AZB remains hindered by the physical and chemical instability of the Zn anode. The Zn anode suffers from dendrite growth and chemical reactions with the electrolyte, leading to efficiency decay and capacity loss. Recently, significant effort has been dedicated to regulating the Zn anode. Electrolyte manipulation, including tailoring the salt, additives, or concentration, is a useful strategy as the electrolyte strongly influences the anode's failure processes. It is thus worthwhile to gain an in‐depth understanding of these electrolyte‐dependent regulation mechanisms. With this in mind, this review first outlines the two main issues behind Zn anode failure, dendrite growth, and side reactions. Subsequently, an understanding of the electrolyte tailoring strategy, namely, the influence of the salt, additive, and concentration on the Zn anode, is provided. We conclude by summarizing the future prospects of the Zn metal anode and potential electrolyte‐based solutions.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/bte2.20220029

Electrolyte engineering strategies for regulation of the Zn metal anode in aqueous Zn‐ion batteries

Combination of alkaline phosphatase/graphene oxide nanoconjugates and D-glucose-6-phosphate-functionalized gold nanoparticles for the rapid colorimetric assay of pathogenic bacteria.

Highly Reversible and Stable Zn Metal Anode under Wide Temperature Conditions Enabled by Modulating Electrolyte Chemistry

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Combination of alkaline phosphatase/graphene oxide nanoconjugates and D-glucose-6-phosphate-functionalized gold nanoparticles for the rapid colorimetric assay of pathogenic bacteria.

Highly Reversible and Stable Zn Metal Anode under Wide Temperature Conditions Enabled by Modulating Electrolyte Chemistry