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首页> 外文期刊>Journal of power sources >Phase field kinetics of lithium electrodeposits
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Phase field kinetics of lithium electrodeposits

机译：锂电沉积物的相场动力学

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摘要

A phase field description is formulated to describe the growth kinetics of an heterogeneously nucleated distribution of lithium electrodeposits. The underlying variational principle includes the bulk electrochemical contributions to the free energy of transformation of the system, the electrolyte-dendrite interfacial energy, and the substrate work of adhesion energetics. Results demonstrate that the rate of electrodeposition at the tip of an isolated dendrite is higher than the rate corresponding to the average overpotential, while the back contact is electrochemically shielded, thus favoring elongated, needle-like shapes. For large populations of electrochemically interacting deposits, two spatially distinct regions of behavior develop: one directly facing the counter-electrode where the local surficial electrodeposition dominates the local kinetics; and a second region, in the vicinity of the substrate-deposit interface, where the electrochemical shielding induced by the tip enables lateral electrochemical lithium exchange dendrite coalescence for small contact angle deposits, and dendrite dewetting and electrodissolution for large contact angle deposits. The underlying physical mechanisms through which some lithium nuclei detach from the depositing substrate, self-induce electrodissolution, while other continue to grow and coalesce are described for different contact angles.
机译：配制了一个相场描述来描述锂电沉积物异相成核分布的生长动力学。潜在的变化原理包括对系统转化自由能的大量电化学贡献，电解质-枝晶界面能以及粘附能的底物功。结果表明，在隔离的枝晶尖端的电沉积速率高于对应于平均超电势的速率，而背面接触被电化学屏蔽，因此有利于细长的针状形状。对于大量的电化学相互作用的沉积物，会形成两个在空间上不同的行为区域：一个直接面对反电极，其中局部表面电沉积主导局部动力学；另一个正对电极。第二区域，在衬底-沉积物界面附近，尖端引起的电化学屏蔽使得侧向电化学锂交换树枝状晶体对于较小的接触角沉积物可以聚结，并且对于较大的接触角沉积物可以进行枝晶去湿和电溶解。对于不同的接触角，描述了一些锂原子从沉积的基底上脱离出来，自我诱导电溶解而其他的继续增长并聚结的潜在物理机制。

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