Understanding and applying coulombic efficiency in lithium metal batteries

Abstract

Coulombic efficiency (CE) has been widely used in battery research as a quantifiable indicator for the reversibility of batteries. While CE helps to predict the lifespan of a lithium-ion battery, the prediction is not necessarily accurate in a rechargeable lithium metal battery. Here, we discuss the fundamental definition of CE and unravel its true meaning in lithium-ion batteries and a few representative configurations of lithium metal batteries. Through examining the similarities and differences of CE in lithium-ion batteries and lithium metal batteries, we establish a CE measuring protocol with the aim of developing high-energy long-lasting practical lithium metal batteries. The understanding of CE and the CE protocol are broadly applicable in other rechargeable metal batteries including Zn, Mg and Na batteries.

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Fig. 1: Various cell configurations and comparisons between CEs and capacity retentions.
Fig. 2: Impacts from Cu substrates, electrolytes and Li on measured CE and observed cycling stability of anode-free NMC batteries.
Fig. 3: Impacts of electrolyte amounts on CE and cycling of Li||Cu and Li||NMC cells.
Fig. 4: A coin cell protocol to measure and interpret CE in LMBs.

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Acknowledgements

This work is based on the discussion results from a workshop on ‘Standards and Protocols for Accelerating the Process from Discovery to Deployment’ held in 2019. This research is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium). PNNL is operated by Battelle for the DOE under contract DE-AC05-76RLO1830.

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Correspondence to Jie Xiao.

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Xiao, J., Li, Q., Bi, Y. et al. Understanding and applying coulombic efficiency in lithium metal batteries. Nat Energy 5, 561–568 (2020). https://doi.org/10.1038/s41560-020-0648-z

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