Dynamic spatial progression of isolated lithium during battery operations

Liu, Fang; Xu, Rong; Wu, Yecun; Boyle, David Thomas; Yang, Ankun; Xu, Jinwei; Zhu, Yangying; Ye, Yusheng; Yu, Zhiao; Zhang, Zewen; Xiao, Xin; Huang, Wenxiao; Wang, Hansen; Chen, Hao; Cui, Yi

doi:10.1038/s41586-021-04168-w

Dynamic spatial progression of isolated lithium during battery operations

Journal Article · Wed Dec 22 00:00:00 EST 2021 · Nature (London)

DOI:https://doi.org/10.1038/s41586-021-04168-w· OSTI ID:1878582

^[1]; Xu, Rong ^[1]; ^[1]; ^[1]; Yang, Ankun ^[1]; Xu, Jinwei ^[1]; Zhu, Yangying ^[1]; ^[1]; ^[1]; Zhang, Zewen ^[1]; ^[1]; Huang, Wenxiao ^[1]; ^[1]; ^[1]; ^[2]

Stanford Univ., CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

The increasing demand for next-generation energy storage systems necessitates the development of high-performance lithium batteries. Unfortunately, current Li anodes exhibit rapid capacity decay and a short cycle life, owing to the continuous generation of solid electrolyte interface and isolated Li (i-Li). The formation of i-Li during the nonuniform dissolution of Li dendrites leads to a substantial capacity loss in lithium batteries under most testing conditions. Because i-Li loses electrical connection with the current collector, it has been considered electrochemically inactive or ‘dead’ in batteries. In this work, contradicting this commonly accepted presumption, we show that i-Li is highly responsive to battery operations, owing to its dynamic polarization to the electric field in the electrolyte. Simultaneous Li deposition and dissolution occurs on two ends of the i-Li, leading to its spatial progression toward the cathode (anode) during charge (discharge). Revealed by our simulation results, the progression rate of i-Li is mainly affected by its length, orientation and the applied current density. Moreover, we successfully demonstrate the recovery of i-Li in Cu–Li cells with >100% Coulombic efficiency and realize LiNi_0.5Mn_0.3Co_0.2O₂ (NMC)–Li full cells with extended cycle life.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1878582

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7890 Vol. 600; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Designable ultra-smooth ultra-thin solid-electrolyte interphases of three alkali metal anodes Gu, Yu; Wang, Wei-Wei; Li, Yi-Juan Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03466-8	journal	April 2018
An ultrathin ionomer interphase for high efficiency lithium anode in carbonate based electrolyte Weng, Yu-Ting; Liu, Hao-Wen; Pei, Allen Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-13783-1	journal	December 2019
Synergistic Effects of Salt Concentration and Working Temperature towards Dendrite-Free Lithium Deposition Li, Panlong; Li, Chao; Yang, Yang Research, Vol. 2019 https://doi.org/10.34133/2019/7481319	journal	October 2019

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