水系锌离子电池具有成本低和安全性高等优点，近年来备受研究人员关注。然而，水系锌电的负极核心问题在于其循环稳定性较差，这限制了其在大规模应用中的可行性。这是因为锌负极在循环过程中由于副反应的发生破坏了表面结构，这些副反应包括枝晶生长、析氢反应以及表面腐蚀等。因此，本文通过在锌负极表面涂覆聚合物保护层的策略，来抑制枝晶生长等副反应，以期提高锌负极界面的电化学稳定性。研究内容如下：

聚氧化乙烯(PEO)作为广泛使用的薄膜材料被用作聚合物保护层。为了提高PEO的离子电导率，CeO₂被添加到PEO中。PEO保护层隔离了电解液和金属锌，有效抑制了析氢反应的发生。同时，CeO₂的加入降低了PEO的结晶度，促进了PEO的链段运动，进一步提高了PEO的离子导电率，从动力学上抑制了枝晶的生长。因此，使用CeO₂@PEO胶涂覆的锌负极组装的对称电池在3 mA·cm^-2的电流密度下可以循环1990 h，远高于空白电池(200 h)。与V₂O₅组装的全电池在5 A·g^-1的电流密度下循环1000 圈后放电容量为103 mA h·g^-1。

聚甲基丙烯酸甲酯(PMMA)作为一种具有良好机械性能和结构稳定性的材料，被选为聚合物保护层，以进一步优化锌负极的循环性能。同时，DFT理论表明SiO₂与PMMA的复合效果较好。此外，通过对锌离子在界面中的输运进行分析，超薄涂层通过减少锌离子传输路径，显著的降低了电池阻抗，并进一步提高锌离子的迁移速率。因此，具有SiO₂@PMMA超薄保护层的对称电池在3 mA·cm^-2的电流密度下具有2200 h的循环寿命，并且在剥离/沉积过程中保持良好的稳定性。此外，全电池在5 A·g^-1的电流密度下循环1000 圈后放电容量为121 mA h·g^-1。

聚乙烯醇(PVA)作为一种可以与锌负极产生良好黏附性的聚合物被选为锌负极保护层。通过与聚丙烯酸(PAA)复合从而形成具有双网络结构的聚合物复合保护层。PVA可以通过羟基调节锌离子的沉积过程，而PAA柔性网络与PVA网络复合后可形成双网络结构，增强复合保护层的性能。此外，通过DFT理论对PVA@PAA复合结构进行分析，PAA能够提高PVA的反应活性，从而促进锌离子在复合涂层中的传输速率。因此，所构建的PVA@PAA双网络超薄界面保护层有助于实现均匀的锌离子沉积，从而实现稳定的锌负极。对称电池展现出长达2400 h的超长循环寿命。全电池在5 A·g^-1的电流密度下稳定循环1000 圈后放电容量为111.3 mA h·g^-1。通过使用改性聚合物保护层对锌负极进行涂覆，实现稳定的锌负极，优化了电池的循环稳定性。改性聚合物的填料能够降低聚合物的结晶度，从而提高其机械性能和离子电导率，进而实现良好的保护效果。

Aqueous zinc ion batteries have attracted much attention from researchers in recent years due to their low cost and high safety. However, the core problem with the anode of aqueous zinc ion batteries is its poor cycling stability, which limits its feasibility for large-scale applications. This is because the surface structure of the zinc anode is damaged during the cycling process due to the occurrence of side reactions, which include dendrite growth, hydrogen evolution reaction, and surface corrosion. Therefore, in this paper, a polymer protective layer is coated on the surface of zinc anode to inhibit the side reactions, including dendrite growth, with a view to improving the electrochemical stability of the zinc-anode interface. The main results of those study are as follows:

Polyethylene oxide (PEO) is used as a widespread film material as a polymer protective layer. In order to improve the ionic conductivity of PEO, CeO₂ was introduced into PEO. The PEO protective layer isolated the electrolyte and metallic zinc, effectively inhibiting the occurrence of hydrogen evolution reaction. Meanwhile, the addition of CeO₂ reduced the crystallinity of PEO, promoted the chain segment movement of PEO, further improved the ionic conductivity of PEO, and kinetically inhibited the growth of dendrites. As a result, the symmetric battery assembled with CeO₂@PEO electrode was cycled for 1990 h at a current density of 3 mA·cm^-2, which was much higher than that of the blank battery (200 h). The full battery assembled with V₂O₅ had a discharge capacity of 103 mA h·g^-1 after 1000 cycles at a current density of 5 A·g^-1.

Polymethyl methacrylate (PMMA), a material with good mechanical properties and structural stability, was selected as the polymer protection layer to further optimize the cycling performance of the zinc anode. Meanwhile, the DFT theory showed that the composite effect of SiO₂ and PMMA was better. In addition, by analyzing the transport of zinc ions in the interface, the ultrathin coating significantly reduces the battery impedance and further improves the migration rate of zinc ions by reducing the zinc ion transport path. Thus, the symmetric battery with SiO₂@PMMA protective layer has a cycle life of 2200 h at a current density of 3 mA·cm^-2 and maintains good stability during the plating/stripping process. Furthermore, the discharge capacity of the full battery was 121 mA h·g^-1 after 1000 cycles at a current density of 5 A·g^-1.

Polyvinyl alcohol (PVA) was selected as a polymer that can produce good adhesion with zinc anode as a protective layer for zinc anode. The polymer composite layer with ultrathin and dual network structure was formed by compositing with polyacrylic acid (PAA), which could regulate the plating process of zinc ions through hydroxyl groups, and the flexible network of PAA could be composited with the network of PVA to form a dual-network structure, which could enhance the performance of composite protective layer. In addition, the PVA@PAA composite structure was analyzed by DFT theory, and PAA could increase the reactivity of PVA, thus promoting the transport rate of zinc ions in the composite coating. Therefore, the constructed PVA@PAA dual-network ultrathin interfacial protective layer contributes to the uniform deposition of zinc ions, resulting in a stable zinc anode. The symmetrical battery exhibits an ultra-long cycle life of up to 2400 h. The discharge capacity of the full battery was 111.3 mA h·g^-1 after 1000 cycles at a current density of 5 A·g^-1. Through the use of a modified polymer protective layer to coat the zinc anode, a stable zinc anode is achieved, optimizing the cycle stability of the battery during cycling. The filler of the modified polymer reduces the crystallinity of the polymer, which improves its mechanical properties and ionic conductivity, thus achieving good protection.

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