Thermodynamic Overpotentials and Nucleation Rates for Electrodeposition on Metal Anodes

• DOI: 10.1021/acsami.8b19787
• Publication Date: 2019-01-30T19:02:59Z
• Authors: Kyle S. Nagy; Saeed Kazemiabnavi; Katsuyo Thornton; Donald J. Siegel
• Keywords: Overpotential; Stripping (fiber); Plating (geology)

Rechargeable batteries employing metal negative electrodes (i.e., anodes) are attractive next-generation energy storage devices because of their greater theoretical densities compared to intercalation-based anodes. An important consideration for a metal's viability as an anode is the efficiency with which it undergoes electrodeposition and electrodissolution. The present study assesses thermodynamic deposition/dissolution efficiencies associated nucleation rates seven metals (Li, Na, K, Mg, Ca, Al, Zn) relevance battery applications. First-principles calculations were used evaluate overpotentials at terraces steps on several low-energy surfaces these metals. In general, observed be smallest plating/stripping largest terrace sites. difference in coordination number surface atom from that bulk was found correlate overpotential magnitude. Consequently, low coordination, body-centered alkali K) predicted among most thermodynamically efficient plating/stripping. contrast, larger such Zn, alkaline earths (Ca Mg) generally exhibit higher overpotentials. rate steady-state during estimated using classical model informed by first-principles calculations. Nucleation orders magnitude than other This multiscale highlights sensitivity behavior structure composition electrode surface.