水系可充电锌离子电池因其本征安全、低成本、无毒和锌具有合适的氧化还原电位等优势，引起广泛关注，被认为是在大规模储能应用中有潜力的候选者。负极材料作为电池的重要组成部分，是实现高性能锌离子电池的关键因素之一。锌离子电池负极主要分为非金属负极和锌金属基负极两大类。其中非金属负极能够避免枝晶生长和析氢等副反应，但面临高的制备成本和低的锌离子扩散动力学、较高的氧化还原电位等问题；锌金属基负极具有低的氧化还原电位和高的比容量，但面临枝晶生长、析氢和腐蚀等副反应的巨大挑战。针对这些问题，本论文以制备无枝晶高性能锌离子电池负极为导向，在制备和研究高性能非金属负极材料的同时，也研究金属负极的高效改性策略（表面改性、界面重构、电解液调控），为实现高性能水系可充电锌离子电池提供多重保障。此外，本论文还通过电化学分析、原位表征和理论计算相结合的方式揭示性能提升机制。本文的主要成果如下：

（1）1,4,5,8-萘二酰亚胺（NI）有机材料作为锌离子电池负极时，在循环过程中会发生溶解和电极结构劣化等问题导致电池性能衰退。为了提升电极结构的稳定性，本章通过调控粘结剂和制备工艺对NI电极进行处理，发现使用聚四氟乙烯（PTFE）粘结剂及辊压工艺制备的NI电极（RNI-PTFE）显示出最优异的电化学性能。当电流密度为3 A g^-1时，RNI-PTFE电极在循环2200圈后仍显示出高达123.3 mA h g^-1的放电容量。结合原位/非原位表征手段揭示了NI电极的离子存储机制及性能增强原理，将这种策略应用于其他有机物中也实现了性能显著提升，表明这种策略具有普适性。此外，基于普鲁士蓝（KZnHCF）正极和RNI-PTFE负极组装的全电池显示出优异的倍率性能（在电流密度为10 A g^-1时放电比容量为113.9 mA h g^-1）、～1.2 V的平均放电电压和50.2 Wh kg^-1的能量密度（电流密度为1 A g^-1）。这项工作为开发高性能水系锌离子电池无枝晶有机负极提供新的设计策略。

（2）由于锌金属在水系电解液中热力学不稳定，活性水分子会腐蚀锌负极导致寄生反应发生。本章利用原子层沉积（ALD）技术在锌金属表面构筑一层不同厚度的ZrO₂界面层（ZrO₂@Zn），其中厚度为40 nm的ZrO2@Zn电极具有最佳的综合性能。40 nm ZrO₂@Zn//40 nm ZrO2@Zn对称电池在1 mA cm^-2 / 0.5 mA h cm^-2条件下显示出低的极化（36 mV）和长的寿命（1750 h）。即使电流密度提升到10 mA cm^-2时，该对称电池依然能够稳定循环860 h，实现高达4.3 Ah cm^-2的累计沉积容量。40 nm ZrO₂@Zn//40 nm ZrO₂@Cu非对称电池也显示出优异的可逆性。此外，根据COMSOL模拟和电化学结果表明，ZrO₂镀层能够隔绝水与锌负极的接触从而抑制寄生副反应，并能够匀化界面电场促进锌离子均匀沉积和抑制枝晶生长，从而实现优异的可逆性和循环稳定性。此外，基于二氧化锰（MnO₂）正极和40 nm ZrO₂@Zn负极组装的全电池在3.08 A g^-1的电流密度下循环2500圈后仍展现出高达137.7 mA h g^-1的放电容量。

（3）在水系电解液中，锌金属负极表面随机分布的氧化层会加速金属锌的钝化和不均匀沉积，严重阻碍了水系锌离子电池走向实际应用。本章重新揭示了氧化层（ZnO）对锌负极的作用，并证明了表面终止行为对提升水系锌离子电池电化学性能的重要性。ZnO层会演化成均匀分布的羟基硫酸锌（Zn₄(OH)₆SO₄·xH₂O，ZSH）保护层，这种保护层并没有直接参与锌的沉积/溶解过程，而是具有降低脱溶剂化能和保护锌负极的作用。通过实验和模拟相结合，提出并验证了一种“边缘脱水-沿边缘转移”的锌离子输运新机制，明确区别于“表面脱水-晶体通道转移”传统机制。由于锌枝晶生长和副反应得到有效抑制，ZnO@Zn//ZnO@Zn对称电池在电流密度为10 mA cm^-2时表现出超过1200 h的稳定寿命以及高达6.24 Ah cm^-2的累积沉积容量，远优于Zn//Zn对称电池。此外，基于MnO₂正极和ZnO@Zn负极组装的全电池展现出超1000圈的优异循环稳定性及高达99.07%的库伦效率。该工作表明合适的表面终止化学设计对于提高金属负极性能是至关重要的。

（4）电解液添加剂策略具有低成本、易操作等优势而被广泛研究。本章将谷氨酸钠添加剂引入硫酸锌电解液中（MSG/ZnSO₄），实现了锌负极表面固态电解质界面（SEI）保护层的构筑，从而提升了锌负极的可逆性和稳定性。根据理论计算和实验分析，发现谷氨酸阴离子（Glu^-）会优先吸附在锌金属表面，并在沉积过程中发生还原反应形成稳定的SEI层，从而有效抑制了锌负极界面处的副反应和提高了锌负极的电化学动力学。因此，使用MSG/ZnSO₄电解液的Zn//Zn对称电池展示出长达4000 h的循环寿命，Zn//Cu电池能够可逆循环1350圈，且平均库伦效率高达99.35%，MnO₂//Zn全电池在1300圈循环后比容量仍然高达108.7 mA h g^-1。该工作中展示的原位SEI设计新策略为实现锌的有效利用以及ZIBs的内在安全性和稳定性开辟了一种高效且廉价的新途径。

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