The morphologies metal electrodeposits adopt during the earliest stages of electrodeposition at planar or non-planar interfaces are known to influence the reversibility of electrochemical cells that use metals as anodes. Viscoelastic interphases — whether formed unintentionally (<i>e.g.</i> by physical adsorption of long-chain polymer additives from complex fluid  electrolytes, by chemical reaction of electrolyte components in contact with a reactive metal electrode), or deliberately (<i>e.g</i>. by creating linear or cross-linked polymer coatings on a metal or ion-selective membrane) are likewise known to have profound effects on electrokinetics at liquid/solid boundaries and on electrodeposit morphology. This talk will discuss results from a combined theoretical and experimental study that seeks to elucidate the effects of interphase chemistry and mechanics on the early-stage nucleation and growth of electrodeposited lithium. Through comparisons of Li nucleation and growth dynamics in simple and complex fluid electrolytes it will be shown that a sufficiently comprehensive picture of the initial nucleation and growth dynamics emerges to enable purposeful design of Artificial Solid Electrolyte Interphases (ASEI) for achieving reversible metal electrodeposition. I will show further that ion diffusion in the bulk electrolyte and through the Solid Electrolyte Interphase (SEI) formed on the metal play equally important roles in early stage nucleation and growth, and that sluggish interfacial transport is an important source of irreversibility at reactive metal electrodes.

Analyzing nucleation and early-stage growth of metal electrodeposits in simple and complex fluid electrolytes

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.