金属电极的苔藓状生长：竞争法拉第反应和快速充电的作用
Moss-like growth of metal electrodes: On the role of competing faradaic reactions and fast-charging
摘要：
在液体电解质中的活性金属的电还原期间不受控制的晶体生长产生多孔的、低密度的、苔藓状的金属沉积物，其主要沿着平面电极基板的表面法向矢量生长。苔藓状沉积物是脆弱的，并通过化学、物理和机械途径导致电池过早失效。在这里，我们使用电分析旋转圆盘电极（RDE）在三电极电化学电池的研究，以阐明苔藓状生长的金属的根本起源。我们报告说，竞争法拉第反应发生在电极表面上的现象的来源。在此基础上，我们得出结论，苔藓状生长制度可以访问任何金属的电沉积过程中的电解质化学和沉积速率的微妙变化。具体地，对于Zn，一种通常不知道形成苔藓状电沉积物的金属，在强碱性电解质中在低电流密度下出现明显的苔藓状沉积图案，所述强碱性电解质经历电还原以在电沉积的Zn上形成界面。相反，我们发现，在金属电镀的速率相对于其他竞争法拉第反应的速率较大的条件下，有可能消除Zn的苔藓状生长机制。总之，我们的研究结果开辟了一种新的方法，可以在使用金属阳极的下一代电池中同时实现良好的金属沉积形态和快速充电。
英文摘要：
Uncontrolled crystal growth during electroreduction of reactive metals in liquid electrolytes produces porous, low-density, mossy metal deposits that grow primarily along the surface normal vector to a planar electrode substrate. The moss-like deposits are fragile and cause premature failure of batteries by chemical, physical, and mechanical pathways. Here we use electroanalytical Rotating-Disk Electrode (RDE) studies in a three-electrode electrochemical cell to elucidate the fundamental origin of moss-like growth of metals. We report that competing Faradaic reactions occurring on the electrode surface is the source of the phenomenon. On this basis, we conclude that a moss-like growth regime can be accessed during electrodeposition of any metal by subtle shifts in electrolyte chemistry and deposition rate. Specifically, for Zn, a metal that conventionally is not known to form moss-like electrodeposits, obvious moss-like deposition patterns emerge at low-current densities in strongly-alkaline electrolytes that undergo electroreduction to form an interphase on the electrodeposited Zn. Conversely, we find that under conditions where the rate of metal electroplating is large relative to that of other competing Faradaic reactions, it is possible to eliminate the mossy-like growth regime for Zn. Taken together, our findings open up a new approach for simultaneously achieving favorable metal deposition morphology and fast charging in next-generation batteries using metal anodes.
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