Abstract Solid polymer electrolytes (SPEs) and hydrogel electrolytes were developed as electrolytes for zinc ion batteries (ZIBs). Hydrogels can retain water molecules and provide high ionic conductivities; however, they contain many free water molecules, inevitably causing side reactions on the zinc anode. SPEs can enhance the stability of anodes, but they typically possess low ionic conductivities and result in high impedance. Here, we develop a lean water hydrogel electrolyte, aiming to balance ion transfer, anode stability, electrochemical stability window and resistance. This hydrogel is equipped with a molecular lubrication mechanism to ensure fast ion transportation. Additionally, this design leads to a widened electrochemical stability window and highly reversible zinc plating/ stripping. The full cell shows excellent cycling stability and capacity retentions at high and low current rates, respectively. Moreover, superior adhesion ability can be achieved, meeting the needs of flexible devices. 

https://www.nature.com/articles/s41467-023-39634-8.pdf

Lean-water hydrogel electrolyte for zinc ion batteries

The in-depth understanding of the composition-property-performance relationship of solid electrolyte interphase (SEI) is the basis of developing a reliable SEI to stablize the Zn anode-electrolyte interface, but it remains unclear in rechargeable aqueous zinc ion batteries. Herein, a well-designed electrolyte based on 2M Zn(CF3SO3)2-0.2M acrylamide-0.2M ZnSO4 is proposed. A robust polymer (polyacrylamide)-inorganic (Zn4SO4(OH)6.xH2O) hybrid SEI is in-situ constructed on Zn anodes through controllable polymerization of acrylamide and coprecipitation of SO42- with Zn2+ and OH-. For the first time, the underlying SEI composition-property-performance relationship is systematically investigated and correlated. The results showed that the polymer-inorganic hybrid SEI, which integrates the high modulus of the inorganic component with the high toughness of the polymer ingredient, can realize high reversibility and long-term interfacial stability, even under ultrahigh areal current density and capacity (30 mA cm-2 ~ 30 mAh cm-2). The resultant Zn||NH4V4O10 cell also exhibits excellent cycling stability. This work will provide a guidance for the rational design of SEI layers in rechargeable aqueous zinc ion batteries.

Rational Design of An In-Situ Polymer-Inorganic Hybrid Solid Electrolyte Interphase for Realising Stable Zn Metal Anode under Harsh Conditions.

Solid polymer electrolyte‐based batteries show great promise because of their safe operating properties, wide voltage window and suitable flexibility. However, low ionic conductivity, low cation transfer number, weak oxidation/reduction resistance and low mechanical strength limit their implementation in Zn ion batteries. Here, w e developed a “polymer‐in‐salt” Zn2+‐conductive solid electrolyte (denoted as 70% salt‐SPE) constructed by a simple and fast phase transition method. The room‐temperature ionic conductivity and the transfer number of the 70% salt‐SPE reaches 1.6 mS cm−1 and 0.78, respectively. Meanwhile, the ZnF2‐rich inorganic/organic hybrid solid electrolyte interface is formed, and the stable voltage window reaches 9.35 V. In consequence, the Zn||Zn symmetric cell continuously cycles over 700 hours at current density of 2 mA cm−2 and the Zn||Cu symmetric battery runs with Coulombic efficiency of >99%. The Zn||MnPBA full battery delivers a discharge specific capacity of 109 mAh g−1 at room temperature and 190 mAh g−1 at 60 °C. Meanwhile, impressive cyclic stability of 6000 cycles with capacity retention of 80% is achieved, which originates from the effectively optimized ion transport action and dendrite‐free Zn plating/stripping.

A “Polymer‐in‐Salt” Solid Electrolyte Enabled by Fast Phase Transition Route for Stable Zn Batteries

Roles of electrolyte additive in Zn chemistry

Zinc-ion batteries (ZIBs) have been attracting much interest as metallic Zn anodes have high theoretical capacity and low redox potential. However, the practical use of ZIBs are severely hampered by...

Advances and Strategies of Electrolyte Regulation in Zn-ion Batteries

Solid polymer electrolytes (SPEs) offer a viable path for overcoming the interfacial problems caused by side reactions and irregular deposition in rechargeable Zn (zinc)–metal batteries. However, this potential has been hampered by limited Zn2+ mobility in polymers; a central conundrum remains on how to solvate Zn2+ strongly enough to free it from anionic traps but weakly enough to minimize its migration barriers. Inspired by biologically dynamic Zn functions, we report a general strategy for constructing highly Zn2+-conductive SPEs by the engineering of heteroleptic coordination. Leveraging polymerization catalyzed by Lewis-acidic Zn2+ predissociated eutectics, we stoichiometrically integrate polymeric ligands (polyacrylamide) with kindred small-molecule co-ligands (acetamide) for Zn2+ centers. This heteroleptic configuration allows for the formation of entropy-increased ion channels with both labile Zn2+–polymer bonding and accelerated polymer mobility, warranting conductivity gains of 2 orders of magnitude and doubling the Zn2+-transference number to 0.44, compared with traditional SPEs. The applicability of the proposed heteroleptic coordination design is also demonstrated by the improved reversibility of Zn plating/stripping process (1200 h) and prolonged cycle life of solid Zn–metal batteries (350 cycles with Mo6S8 cathodes) with improved Coulombic efficiency (∼99%). This study underscores the importance of tailoring the coordination environment in improving cationic mobility in polymers. 

Heteroleptic Coordination Polymer Electrolytes Initiated by Lewis-Acidic Eutectics for Solid Zinc–Metal Batteries

Studying the characteristics and molecular mechanisms of liquid self-diffusion coefficient and viscosity changes is of great significance for, e.g., chemical and petroleum processing. As an example of a highly complex liquid, asphaltene-free high-acid and high-viscosity crude oil and its extracted fractions were studied by comparing their 1H DOSY diffusion maps. The crude oil exhibited a polydisperse diffusion distribution, including multiple diffusion portions with diffusion coefficients much smaller than that of any single fraction in independent diffusion. The main mechanism that leads to the decreases in the diffusion coefficients of crude oil is attributed to diffusion resistance enhanced by Dynamical Molecular-Interaction Networks (DMINs), rather than by enlargement of the diffusion species caused by molecular aggregation. Constructed through the synergistic interactions of various polar molecules in crude oil, DMINs dynamically bind polar molecules, trap polarizable molecules, and spatially hinder the free motion of non-polar molecules. Overall, this reduces the diffusion coefficients of all molecular. This study demonstrates that DOSY is a powerful NMR method to investigate molecular motion abilities in complex mixtures. In addition, the insights in the influence of the interaction matrix on the molecular mobility also help to understand the contribution of "structural viscosity" to the viscosity of heavy oil.

Diffusion-Ordered Spectroscopy (DOSY) as a Powerful NMR Method to Investigate Molecular Mobities and Intermolecular Interactions in Complex Oil Mixtures.

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Heteroleptic Coordination Polymer Electrolytes Initiated by Lewis-Acidic Eutectics for Solid Zinc–Metal Batteries

Diffusion-Ordered Spectroscopy (DOSY) as a Powerful NMR Method to Investigate Molecular Mobities and Intermolecular Interactions in Complex Oil Mixtures.