柔性锌离子电池水凝胶电解质研究进展

doi:10.6023/cjoc202306015

摘要/Abstract

为了满足多样化的柔性可穿戴电子设备的发展, 需要与之相匹配的供能系统. 柔性锌离子电池因其安全性高、易组装及能量密度高等特点受到广泛关注, 而水凝胶电解质则是柔性锌离子电池中的重要组成部分, 因此受到广泛研究. 综述了水凝胶电解质的可控构筑方法, 详细总结了柔性锌离子电池水凝胶电解质的最新研究成果, 包括力学增强型、自愈合型、低温型和环境响应型水凝胶电解质. 此外, 还对高性能水凝胶电解质的未来发展进行了展望.

关键词: 水凝胶电解质, 柔性锌离子电池, 力学增强, 自愈合, 低温, 环境响应

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

引用此文

章炜, 夏欢, 曹昕, 徐彬瑜, 李峥沄. 柔性锌离子电池水凝胶电解质研究进展[J]. 有机化学, 2024, 44(1): 148-158.

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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图/表 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

表1. 水凝胶电解质常用高分子网络材料的分子结构及其一般特征[34]

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]

表2. 常见水凝胶电解质离子性能与力学性能

Table 2. Ionic and mechanical properties of common hydrogel electrolytes

图1. (a) HPE的合成路线示意图及(b~e)固态可充电ZIB在不同破坏试验中的电化学性能[71]

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.

图2. (a)自愈合ZIBs结构示意图, (b)在切割前(开灯)、切割后(关灯)以及自愈后(再次开灯)两个自愈ZIBs串联为包含23个灯泡的LED阵列供电的照片, (c)环境条件下PVA-COOH水凝胶电解质的自愈行为, 以及(d)通过切割/自愈操作切换为LED灯泡供电[74,77]

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]

图3. (a) PDC-20凝胶电解质的制备方案、(b) PDC-20凝胶电解质交联反应机理以及(c~k)在－40 ℃条件下经过一系列破坏实验的柔性ZIBs的电化学性能[78-79]

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 ℃.

图4. (a) Pluronic 水凝胶电解质(PHE)冷却-恢复过程示意图、(b)不同温度下PHE和相应聚合物链构型的图片(插图)、(d, e)随冷却时间(－5 ℃)的变化PHE对Zn电极表面的润湿行为、(c)空白锌电极和(f)被PHE完全润湿的锌电极的扫描电子显微镜(SEM)横截面图、(g) WO3阴极插入Al3＋时锌阳极发生Zn/Zn2＋氧化还原反应的双层器件示意图以及(h)以过硫酸钾为引发剂, N,N'-亚甲基双丙烯酰胺为交联剂, 以丙烯酰胺为原料合成聚丙烯酰胺的一般工艺流程[81,84]

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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