锌离子电池电解液添加剂设计及锌负极保护机理研究

当今世界能源与环境问题日益严峻，基于锂离子电池的能量存储系统具有高效存储和转换能量的特性，已在电子设备、电动汽车及储能电网等领域占据了主导地位。然而，目前仍然存在资源短缺、成本高以及安全性差等问题限制了锂离子电池的发展。水系锌离子电池由于容量高、制作流程简单、安全廉价等特点而受到广泛关注，但是枝晶生长、锌腐蚀、副反应等难以避免的问题使得金属锌负极的长期循环稳定性较差、库伦效率较低，严重阻碍了锌的大规模应用。目前，引入电解液添加剂是改善锌负极结构稳定性最简便、最经济的方法。本论文设计了一种糖类添加剂改性锌负极的策略，通过对比含有不同种类及官能团数量的糖类添加剂，深入分析其对锌负极的界面化学以及电化学性能的影响，最终研发出了具有高稳定性的锌离子电池。具体研究内容如下：

首先，通过VASP软件分析了不同糖类小分子与锌表面吸附能、差分电荷密度，并且通过COMSOL软件利用有限元分析对锌枝晶的生长进行模拟，研究结果表明：糖类小分子添加剂可以吸附在锌负极表面，屏蔽部分尖端效应的影响，限制Zn²⁺在界面处的不可控的二维扩散行为，使得锌能够沉积得更加均匀，从而缓解枝晶生长。其中糖类分子的羟基与锌金属之间电子云密度分布较大，说明吸附作用主要源于羟基与锌直接的库伦作用。因此，相比于单糖，蔗糖与锌金属间电子云分布更广，吸附能力更强。

其次，通过对不同种类和浓度的糖类小分子添加剂进行电化学性能测试，并对电解液、极片等进行表征分析进一步验证其对锌负极改性机理，研究结果表明：在电流密度为0.5 mA cm^-2，比容量为0.5 mAh cm^-2下，引入10mM蔗糖添加剂的Zn//Zn对称电池可以稳定1300h以上，100mM稳定循环时间达到了2000多个小时，全电池在近900次循环后容量保持率达到85%。ZnSO₄电解质中引入糖类小分子可以改变Zn²⁺的六水溶剂化结构，削弱Zn²⁺和硫酸根离子之间的静电相互作用，提高界面稳定性，有效抑制副反应的发生、产气等问题，使得锌负极电化学性能得到优化。

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