Research Progress on Hydrogel Electrolytes for Flexible Zinc-Ion Batteries

doi:10.6023/cjoc202306015

Abstract

To meet the development of diverse flexible wearable electronic devices, a corresponding power supply system is needed. Flexible zinc-ion batteries have been widely studied due to their high safety, easy assembly, and high energy density. As an important component of flexible zinc-ion batteries, hydrogel electrolytes have been widely studied. The controllable construction methods of hydrogel electrolytes are introduced. The latest research achievements of multifunctional hydrogel electrolytes for flexible zinc-ion batteries, mainly including mechanically enhanced, self-healing, low-temperature, and environmental response hydrogel electrolytes, are summarized in detail. In addition, the future development of high-performance hydrogel electrolytes is also prospected.

Key words: hydrogel electrolyte, flexible zinc-ion battery, mechanical enhancement, self-healing, low-temperature, environmental response

Cite this article

Wei Zhang, Huan Xia, Xin Cao, Binyu Xu, Zhengyun Li. Research Progress on Hydrogel Electrolytes for Flexible Zinc-Ion Batteries[J]. Chinese Journal of Organic Chemistry, 2024, 44(1): 148-158.

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Fig. & Tab. 6

水凝胶名称	官能团	交联方式
聚乙烯醇	羟基	物理交联
聚丙烯酸	羧基	离子交联
聚丙烯酰胺	酰胺基	自由基交联
明胶	肽键、羟基	物理交联
海藻酸	羟基、羧基	离子交联
琼脂糖	羟基、醚键	物理交联
壳聚糖	羟基、氨基、醚键	化学交联

Table 1. Molecular structures and general characteristics of polymer network materials commonly used in hydrogel electrolytes[34]

水凝胶	离子电导率/(mS•cm^－1)	力学性能	参考文献
聚乙烯醇	8.97	可弯曲(0~180°)	[65,70]
黄原胶	16.5	—	[66]
明胶	6.15	可弯曲、可扭曲、可卷曲, 可剪切及水下工作	[67]
羧甲基纤维素	—	可弯曲(0~180°), 90°弯曲(>3000次)	[68]
聚丙烯酰胺	—	可拉伸(1400%~3000 %), 可压缩(0~80 %)	[69]
分层结构(PAM-PAN-Gelatin)	17.6	可弯曲、可扭曲、可卷曲, 最大拉应力7.76 MPa	[71]
聚两性离子(Zwitterionic Sulfobetaine)	24.6	可拉伸(920%)	[39,72]

Table 2. Ionic and mechanical properties of common hydrogel electrolytes

Figure 1. (a) Schematic of the synthesis route to the HPE and (b~e) electrochemical performances of the solid-state rechargeable ZIB in different destructive tests[71] The hierarchical structured HPE was synthesized by grafting PAM on gelatin chains that are filled in the network of PAN electrospun fiber membrane through a facile free radical polymerization approach. (b) Bending test. (c) Hammering test. (d) Washing test. (e) Drilling test.

Figure 2. (a) Illustration of the structure of self-healing integrated all-in-one ZIBs, (b) photographs of the two self-healing ZIBs in series powering an LED array containing 23 bulbs before cutting (light on), after cutting (light off) and after self-healing with dislocation in the direction parallel to the surface of devices (light on again), (c) self-healing behaviors of the PVA-COOH hydrogel electrolyte under ambient conditions, and (d) switching of an LED bulb through cut/self-healing operations[74,77]

Figure 3. (a) Preparation scheme of PDC-20 gel electrolyte, (b) mechanistic of the cross-linking reaction of PDC-20 gel electrolyte, and (c~k) electrochemical performance of the flexible ZIBs undergoing a series of destructive experiments at －40 ℃[78-79] (c) Scheme of the bending state of the flexible ZIBs. Electrochemical performance of flexible ZIBs at 5 A?g－1 current density under (d) bending, (e) squeezing, folding, and twisting mechanical deformation. (f~j) Demonstration of powering a timer under different deformation conditions at －40 ℃: bending, folding, twisting, rolling and compressing. (k) Three ZIBs were connected in series and mounted on a prosthetic wrist, powering an electronic bracelet at －40 ℃.

Figure 4. (a) Cooling-recovery function by incorporation of a thermoreversible Pluronic hydrogel electrolyte (PHE); (b) photographs of PHE and corresponding polymer chain configurations (insets) at different temperatures; (d, e) wetting behavior of Zn electrode surface with PHE during evolution of cooling time (－5 ℃); cross-sectional scanning electron microscope (SEM) images of (c) the blank Zn electrode and (f) the Zn electrode fully wetted by PHE; (g) schematic of the proposed double layer device with Al3＋ intercalation at the WO3 cathode and Zn/Zn2＋ redox reaction at the zinc anode; (h) general synthesis procedure of polyacrylamide from acrylamide with potassium persulfate as the initiator and N,N'-methylenebisacrylamide as the cross linker[81,84]

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