Dynamic spatial progression of isolated lithium during battery operations

Fang Liu, Rong Xu, Yecun Wu, David Thomas Boyle, Ankun Yang, Jinwei Xu, Yangying Zhu, Yusheng Ye, Zhiao Yu, Zewen Zhang, Xin Xiao, Wenxiao Huang, Hansen Wang, Hao Chen and Yi Cui ()
Additional contact information
Fang Liu: Stanford University
Rong Xu: Stanford University
Yecun Wu: Stanford University
David Thomas Boyle: Stanford University
Ankun Yang: Stanford University
Jinwei Xu: Stanford University
Yangying Zhu: Stanford University
Yusheng Ye: Stanford University
Zhiao Yu: Stanford University
Zewen Zhang: Stanford University
Xin Xiao: Stanford University
Wenxiao Huang: Stanford University
Hansen Wang: Stanford University
Hao Chen: Stanford University
Yi Cui: Stanford University

Nature, 2021, vol. 600, issue 7890, 659-663

Abstract: Abstract The increasing demand for next-generation energy storage systems necessitates the development of high-performance lithium batteries1–3. Unfortunately, current Li anodes exhibit rapid capacity decay and a short cycle life4–6, owing to the continuous generation of solid electrolyte interface7,8 and isolated Li (i-Li)9–11. The formation of i-Li during the nonuniform dissolution of Li dendrites12 leads to a substantial capacity loss in lithium batteries under most testing conditions13. Because i-Li loses electrical connection with the current collector, it has been considered electrochemically inactive or ‘dead’ in batteries14,15. Contradicting this commonly accepted presumption, here 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.

Date: 2021
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DOI: 10.1038/s41586-021-04168-w

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