Elucidating Interfacial Stability between Lithium Metal Anode and Li Phosphorus Oxynitride via In Situ Electron Microscopy

Hood, Zachary D.; Chen, Xi; Sacci, Robert L.; Liu, Xiaoming; Veith, Gabriel M.; Mo, Yifei; Niu, Junjie; Dudney, Nancy J.; Chi, Miaofang

doi:10.1021/acs.nanolett.0c03438

Elucidating Interfacial Stability between Lithium Metal Anode and Li Phosphorus Oxynitride via In Situ Electron Microscopy

Journal Article · Fri Dec 18 00:00:00 EST 2020 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.0c03438· OSTI ID:1772870

Hood, Zachary D. ^[1]; ^[2]; ^[3]; ^[4]; ^[3]; ^[5]; ^[2]; ^[3]; ^[4]

Georgia Inst. of Technology, Atlanta, GA (United States)
Univ. of Wisconsin, Milwaukee, WI (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of Maryland, College Park, MD (United States)

Li phosphorus oxynitride (LiPON) is one of a very few solid electrolytes that have demonstrated high stability against Li metal and extended cyclability with high Coulombic efficiency for all solid-state batteries (ASSBs). However, theoretical calculations show that LiPON reacts with Li metal. Here, we utilize in situ electron microscopy to observe the dynamic evolutions at the LiPON–Li interface upon contacting and under biasing. We reveal that a thin interface layer (~60 nm) develops at the LiPON–Li interface upon contact. This layer is composed of conductive binary compounds that show a unique spatial distribution that warrants an electrochemical stability of the interface, serving as an effective passivation layer. Our results explicate the excellent cyclability of LiPON and reconcile the existing debates regarding the stability of the LiPON–Li interface, demonstrating that, though glassy solid electrolytes may not have a perfect initial electrochemical window with Li metal, they may excel in future applications for ASSBs.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1772870

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 1 Vol. 21; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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