From Microparticles to Nanowires and Back: Radical Transformations in Plated Li Metal Morphology Revealed via in Situ Scanning Electron Microscopy

Yulaev, Alexander; Oleshko, Vladimir; Haney, Paul; Liu, Jialin; Qi, Yue; Talin, A. Alec; Leite, Marina S.; Kolmakov, Andrei

doi:10.1021/acs.nanolett.7b04518

Title: From Microparticles to Nanowires and Back: Radical Transformations in Plated Li Metal Morphology Revealed via in Situ Scanning Electron Microscopy

Journal Article · 03 February 2018 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.7b04518 · OSTI ID:1485830

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National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Michigan State Univ., East Lansing, MI (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Univ. of Maryland, College Park, MD (United States)

We report that Li metal is the preferred anode material for all-solid-state Li batteries. However, a stable plating and stripping of Li metal at the anode–solid electrolyte interface remains a significant challenge particularly at practically feasible current densities. This problem usually relates to high and/or inhomogeneous Li-electrode–electrolyte interfacial impedance and formation and growth of high-aspect-ratio dendritic Li deposits at the electrode–electrolyte interface, which eventually shunt the battery. To better understand details of Li metal plating, we use operando electron microscopy and Auger spectroscopy to probe nucleation, growth, and stripping of Li metal during cycling of a model solid-state Li battery as a function of current density and oxygen pressure. We find a linear correlation between the nucleation density of Li clusters and the charging rate in an ultrahigh vacuum, which agrees with a classical nucleation and growth model. Moreover, the trace amount of oxidizing gas (≈10^–6 Pa of O₂) promotes the Li growth in a form of nanowires due to a fine balance between the ion current density and a growth rate of a thin lithium-oxide shell on the surface of the metallic Li. Interestingly, increasing the partial pressure of O₂ to 10^–5 Pa resumes Li plating in a form of 3D particles. In conclusion, our results demonstrate the importance of trace amounts of preexisting or ambient oxidizing species on lithiation processes in solid-state batteries.

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Research Organization:: Sandia National Lab. (SNL-CA), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; EE0007803; SC0001160

OSTI ID:: 1485830

Report Number(s):: SAND-2018-11517J; 669387

Journal Information:: Nano Letters, Vol. 18, Issue 3; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 41 works

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Title: From Microparticles to Nanowires and Back: Radical Transformations in Plated Li Metal Morphology Revealed via in Situ Scanning Electron Microscopy

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