Balancing Interfacial Reactions to Achieve Long Cycle Life in High Energy Lithium Metal Batteries

Journal Article · Thu Jul 01 00:00:00 EDT 2021 · Nature Energy

DOI:https://doi.org/10.1038/s41560-021-00852-3· OSTI ID:1821199

Niu, Chaojiang ^[1]; Liu, Dianying ^[1]; Lochala, Joshua A. ^[1]; Anderson, Cassidy S. ^[1]; Cao, Xia ^[1]; Gross, Mark E. ^[1]; Xu, Wu  ^[1]; Zhang, Jiguang  ^[1]; Whittingham, M. Stanley ^[2]; Xiao, Jie ^[1]; Liu, Jun ^[3]

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1. BATTELLE (PACIFIC NW LAB)
2. State University of New York at Binghamton
3. PNNL

Rechargeable lithium (Li) metal batteries have attracted wide attentions as the next generation energy storage technologies. However, simultaneously achieving high cell-level energy density and long cycle life in realistic batteries is still a great challenge. Here we investigate the cell degradation mechanisms of Li||LiNi0.6Mn0.2Co0.2O2 pouch cells using different, but representative cell configurations to understand the fundamental linkage among Li thickness, electrolyte depletion and the structure evolution of solid electrolyte interphase (SEI) layers. Different cell failure modes were discovered when tuning the anode to cathode capacity (N/P) ratio in compatible electrolyte. With a thick-Li anode (N/P ratio = 2.5), initial stable cycling is obtained because of the abundant Li supply from the anode together with an artificially inflated high Coulombic Efficiency, followed by a premature sudden cell death appears due to the enrichment of “ineffective SEI” which does not participate in the electrochemical reactions but keep increasing cell impedance. The anode-free cell (N/P 0:1) displays a steady capacity decay because cathode Li loss dominates from the beginning to the end of cell cycle life. An optimized thin-Li (N/P 1:1) well balances the Li consumption rate with the impedance buildup by minimizing the growth of ineffective SEI layer, thus decelerates cell polarization increasing and extends cycling. Contrary to conventional wisdoms, long cycle life is observed by using ultra thin-Li (20 µm) in balanced cells. A prototype 350 Wh kg-1 pouch cell (2.0 Ah) achieves over 600 long stable cycles with 76% capacity retention without sudden cell death.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1821199
• Report Number(s): PNNL-SA-158492
• Journal Information: Nature Energy, Vol. 6, Issue 7
• Country of Publication: United States
• Language: English