Rapidly Synthesized Single-Ion Conductive Hydrogel Electrolyte for High-Performance Quasi-Solid-State Zinc-ion Batteries.

Single-ion conductive electrolytes can largely eliminate electrode polarization, reduce the proportion of anion migration and inhibit side reactions in batteries. However, they usually suffer from insufficient ion conductivity due to the strong interaction between cations and cationic receptors. Here we report an ultrafast light-responsive covalent organic frameworks (COF) with sulfonic acid groups modification as the acrylamide polymerization initiator. Benefiting from the reduced electrostatic interaction between Zn2+ and sulfonic acid groups through solvation effects, the as-prepared COF-based hydrogel electrolyte (TCOF-S-Gel) receives an ion conductivity of up to 27.2 mS/cm and Zn2+ transference number of up to 0.89. In addition, sufficient hydrogen bonds endow the single-ion conductive TCOF-S-Gel electrolyte to have good water retention and superb mechanical properties. The assembled Zn||TCOF-S-Gel||MnO2 full zinc-ion battery exhibits high discharge capacity (248 mAh/g at 1C), excellent rate capability (90 mAh/g at 10C) and superior cycling performance. These enviable results enlist the instantaneously photocured TCOF-S-Gel electrolyte to be qualified to large-scaled flexible high-performance quasi-solid-state zinc-ion batteries.

Qiu T ，Wang T ，Tang W ，Li Y ，Li Y ，Lang X ，Jiang Q ，Tan H ... -  《-》

Polymeric Single-Ion Conductors with Enhanced Side-Chain Motion for High-Performance Solid Zinc-Ion Batteries.

Zn-based solid polymer electrolytes (SPEs) have enormous potential in realizing high-performance zinc-ion batteries. Polymeric single-ion conductor (PSIC)-based SPEs can largely eradicate anion migration and side reactions of electrodes with decreased polarization, but the ionic conductivity is still unsatisfactory due to the tight localized ion interactions and sluggish chain motion. Herein, by employing the heterocyclic tetrazole as the anionic center of the side chain, a novel PSIC is fabricated with optimized charge delocalization and enhanced side-chain motion. The as-prepared PSIC delivers an ionic conductivity up to 5.4 × 10-4 S cm-1 with an ultrahigh Zn2+ transference number of 0.94. Based on the PSIC, dendrite-free and hydrogen-free Zn plating/stripping cycling (2000 h) is achieved. A further assembled Zn‖V2 O5 battery exhibits superior performances to other solid ZIBs, including a high discharge capacity, excellent rate capability, and long cycling life. In addition, a remarkable shelf-life (90 d), low self-discharge rate, and good temperature adaptability of the solid battery can be achieved benefiting from the high stability of the SPE during operation. The PSIC-based SPEs with advanced ion-transport structure endow solid ZIBs with significant performance improvement, high safety, and durability.

Chen Z ，Wang T ，Hou Y ，Wang Y ，Huang Z ，Cui H ，Fan J ，Pei Z ，Zhi C ... -  《-》

In Situ Polymerization of a Self-Healing Polyacrylamide-Based Eutectogel as an Electrolyte for Zinc-Ion Batteries.

Li X ，Li Z ，Guo Z ，Zhang C ，Xu X ，Tu J ，Wang X ，Gu C ... -  《-》

Realizing an All-Round Hydrogel Electrolyte toward Environmentally Adaptive Dendrite-Free Aqueous Zn-MnO(2) Batteries.

Flexible energy storage devices are at the forefront of next-generation power supplies, one of the most important components of which is the gel electrolyte. However, shortcomings exist, more or less, for all the currently developed hydrogel electrolytes. Herein, a facile and cost-effective method is developed to construct an all-round hydrogel electrolyte by using cotton as the raw material, tetraethyl orthosilicate as the crosslinker, and glycerol as the antifreezing agent. The obtained hydrogel electrolyte has high ionic conductivity, excellent mechanical properties (e.g., high tensile strength and elasticity), ultralow freezing point, good self-healing ability, high adhesion, and good heat-resistance ability. Remarkably, this hydrogel electrolyte can provide a record-breaking high ionic conductivity of 19.4 mS cm-1 at -40 °C compared with previously reported aqueous electrolytes for zinc-ion batteries. In addition, this hydrogel electrolyte can significantly inhibit zinc dendritic growth and parasitic side reactions from -40 to 60 °C. With this hydrogel electrolyte, a flexible quasi-solid-state Zn-MnO2 battery is assembled, which shows remarkable energy densities from -40 to 60 °C. The battery also exhibits outstanding cycling durability and has high endurance under various harsh conditions. This work opens new opportunities for the development of hydrogel electrolytes.

Chen M ，Chen J ，Zhou W ，Han X ，Yao Y ，Wong CP ... -  《-》

Polysaccharide hydrogel electrolytes with robust interfacial contact to electrodes for quasi-solid state flexible aqueous zinc ion batteries with efficient suppressing of dendrite growth.

Flexible aqueous zinc-ion batteries (AZIBs) require high conductive and adhesive hydrogel electrolytes. However, high adhesion tends to hinder ion conduction rate. Herein, we designed a water/glycerol binary solvent coordinating the hydrophilic polymers to reconstruct the water molecules' environment in the hydrogel. As a consequence, the interface adhesion strength between Zn and the hydrogel reached 3.0 kPa and the ionic conductivity was up to 16.8 mS cm-1. In addition, inspired by the slurry electrode preparation method, we developed a simple blade coating technique using a non-Newtonian polysaccharide liquid solution to construct an ultra-thin hydrogel electrolyte in situ on the cathode. The thickness of the obtained hydrogel reached 70 μm, and the ultrathin flexible AZIBs were easily constructed by pasting a Zn anode directly on the adhesive hydrogel, showing the potential of flexible AZIBs scalable assembly. In addition, the Zn//Zn symmetrical cells with the hydrogel electrolyte provided stable cycling performance for over 400 h at 0.1 mA cm-2 with suppressed dendrite growth. The assembled Zn//Polyaniline battery and Zn//V2O5 battery also exhibited excellent capacity retention after cycles. This work has realized the hydrogel electrolyte with high adhesion and conductivity, which has good adaptability to metal electrodes and opened up a new practical way for large-scale assembly of flexible energy storage devices.

Deng Y ，Wu Y ，Wang L ，Zhang K ，Wang Y ，Yan L ... -  《-》