Physical Orphaning versus Chemical Instability: Is Dendritic Electrodeposition of Li Fatal?

Zheng, Jingxu; Tang, Tian; Zhao, Qing; Liu, Xiaotun; Deng, Yue; Archer, Lynden A.

doi:10.1021/acsenergylett.9b00750

Physical Orphaning versus Chemical Instability: Is Dendritic Electrodeposition of Li Fatal?

Journal Article · Thu May 16 00:00:00 EDT 2019 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.9b00750· OSTI ID:1566575

Zheng, Jingxu ^[1]; Tang, Tian ^[1]; Zhao, Qing ^[1]; Liu, Xiaotun ^[1]; Deng, Yue ^[1]; ^[1]

Cornell Univ., Ithaca, NY (United States)

The dendritic electrodeposition of lithium, leading to physical orphaning and chemical instability, is considered responsible for the poor reversibility and premature failure of electrochemical cells that utilize Li metal anodes. Herein we critically assess the roles of physical orphaning and chemical instability of electrodeposited Li on electrode reversibility using planar and non-planar electrode architectures. The non-planar electrodes allow the morphology of electrodeposited Li to be interrogated in detail and in the absence of complications associated with cell stacking pressure. We find that physical orphaning is a key determinant of the poor reversibility of Li. We report further that fiber-like, dendritic electrodeposition is an intrinsic characteristic of Li —irrespective of the electrolyte solvent chemistry. With guaranteed electronic access to prevent physical loss, we finally show that a Li metal electrode exhibits high levels of reversibility (99.4% CE), even when the metal electrodeposits are in obvious, dendritic morphologies. We take advantage of these findings to create high-loading (7 mAh/cm²) Li||LFP full cells with nearly unity N:P ratio and demonstrate that these cells exhibit good reversibility.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2mt); State Univ. of New York (SUNY), Albany, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012673

OSTI ID:: 1566575

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 6 Vol. 4; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Reversible epitaxial electrodeposition of metals in battery anodes Zheng, Jingxu; Zhao, Qing; Tang, Tian Science, Vol. 366, Issue 6465 https://doi.org/10.1126/science.aax6873	journal	October 2019

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