Flexible Zn-Based Batteries with Polymer Electrolyte

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Batteries 2022, 8, 59 13 of 17 (2) especially by reducing the energy density, which is a specific problem that needs to be solved through future research. The mechanical properties of a battery include its intrinsic flexibility, layer cohesion (self-strength), interlayer adhesion, etc. Its flexibility is determined by the Young’s modulus of the battery. When polymer electrolytes are used for the fabrication of battery devices, the Young’s modulus of the electrolyte will largely determine the Young’s modulus of the battery. It should be noted that the electrode materials and the current collectors also need to be considered. The softness of polymer electrolytes (such as the comfort of wearable applications of flexible batteries) and their mechanical strength (tensile limit and impact resistance) represent a trade-off. Therefore, numer- ous researchers have focused on the design of advanced materials and electrolyte configurations to enhance their mechanical strength. For example, a double network structure can be used to enhance mechanical strength, such as in terms of tensile and compressive properties. The flexibility of a physical/chemical crosslinked single network is also satisfactory, but, at present, attention is focused on the whole device (especially the collector). Li et al. have discussed the softness from a device-level perspective [69]. Yang et al. also discussed the softness of the entire Zn-based battery, in which the softness of the electrolyte is often ignored [70]. These concerns indicate that the softness of the electrolyte needs to be considered further. In addition, for polymer-based flexible battery devices, the adhesion between the electrolyte and the layers should be considered to ensure the structural integrity of devices by increasing the adhesion between layers. When working at extremely cold temperatures, the performance of the electrode mate- rials, especially the electrochemical activity and the ion diffusion rate, will inevitably deteriorate, but, to date, this has not received much attention compared to hydrogel electrolytes. Moreover, due to the water splitting that may occur under an electric field, most aqueous Zn-based batteries containing a mild electrolyte only exhibited a narrow voltage window of <2.0 V. Recently developed “water-in-salt” electrolytes could significantly increase the voltage window of aqueous ZIBs to 2.1 V. However, the high cost is hindering implementation at scale. Therefore, the development of hy- drogel electrolytes with a wider electrochemical potential window is to be encouraged for high-voltage aqueous flexible batteries. The ultimate purpose of the development of flexible Zn-based batteries is commercial- ization. However, the persistent issues of zinc dendrite formation and side-reactions, such as HER and corrosion, continue to adversely affect the stability of the Zn anode. In addition, due to the complicated synthesis of electrode materials and the involved chemical modification of hydrogel electrolytes, the fabrication and assembly processes of flexible batteries are not sufficiently simplified with production efficiency need- ing improvement. Advanced manufacturing technologies, such as 3D printing and screen printing can be integrated and applied into the fabrication of high-performance batteries for enhanced efficiency. During daily use as a portable power accessory for wearable electronics, flexible batteries inevitably undergo frequent extreme deformations. The mechanical stability of polymer electrolytes is thus of great significance for the long-term usability of flexible batteries. However, most hydrogel electrolytes are insufficiently durable to endure frequent deformations and external impacts. New technologies for the synthesis of super-tough or fast self-healing polymer electrolytes should be further explored and disseminated. Moreover, due to unavoidable direct contact of wearable batteries with the human body in realistic use, guaranteeing the biocompatibility of polymer electrolytes is also critical for wearable applications. A well-formed SEI can not only improve the compatibility between electrodes and electrolyte to facilitate the rate of ion flow, but can also prevent the cathodes from pulverization and inhibit side-reactions. Additionally, building an artificial SEI with larger specific active surface area could effectively alleviate concentration polarization, (3) (4) (5) (6)

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