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Title: Dynamic spatial progression of isolated lithium during battery operations

Abstract

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 LiNi0.5Mn0.3Co0.2O2 (NMC)–Li full cells with extended cycle life.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1878582
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 600; Journal Issue: 7890; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

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, and Cui, Yi. Dynamic spatial progression of isolated lithium during battery operations. United States: N. p., 2021. Web. doi:10.1038/s41586-021-04168-w.
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. Dynamic spatial progression of isolated lithium during battery operations. United States. https://doi.org/10.1038/s41586-021-04168-w
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, and Cui, Yi. Wed . "Dynamic spatial progression of isolated lithium during battery operations". United States. https://doi.org/10.1038/s41586-021-04168-w. https://www.osti.gov/servlets/purl/1878582.
@article{osti_1878582,
title = {Dynamic spatial progression of isolated lithium during battery operations},
author = {Liu, Fang and Xu, Rong and Wu, Yecun and Boyle, David Thomas and Yang, Ankun and Xu, Jinwei and Zhu, Yangying and Ye, Yusheng and Yu, Zhiao and Zhang, Zewen and Xiao, Xin and Huang, Wenxiao and Wang, Hansen and Chen, Hao and Cui, Yi},
abstractNote = {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 LiNi0.5Mn0.3Co0.2O2 (NMC)–Li full cells with extended cycle life.},
doi = {10.1038/s41586-021-04168-w},
journal = {Nature (London)},
number = 7890,
volume = 600,
place = {United States},
year = {Wed Dec 22 00:00:00 EST 2021},
month = {Wed Dec 22 00:00:00 EST 2021}
}

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