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Lithium platingone of the critical processes in the desired high-energy lithium metal batteriesis accompanied by lithium whisker growth, which causes several problems that prevent the employment of metallic lithium anodes in rechargeable systems. They include low coulombic efficiency, electrolyte consumption, and the risk of short circuits, which can lead to thermal runaway of the battery. In recent years several strategies were suggested to mitigate whisker growth. The mechanism of this process, however, still lacks understanding. Here, we reveal the importance of surface diffusion along grain boundaries in solid lithium. We show that, at first, the plating of lithium onto a lithium substrate is possible as bulk crystal growth with a planar crystallization front for the Li grains with oblique (nonperpendicular to the surface) grain boundaries. Further, the developed compressive stress makes lithium diffusion to the grain base unfavorable, and new grains nucleate at the surface. The latter are the cause of the whisker growth from their roots. These findings indicate that the control of grain-boundary diffusion and grain size and structure paves the way to overcome the nonuniform morphology of plated lithium.

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