Critical Evaluation of Potentiostatic Holds as Accelerated Predictors of Capacity Fade during Calendar Aging

Maxwell C. Schulze, Marco Tulio F. Rodrigues, Josefine D. McBrayer, Daniel P. Abraham, Christopher A. Apblett, Ira Bloom, Zonghai Chen, Andrew M. Colclasure, Alison R. Dunlop, Chen Fang, Katharine L. Harrison, Gao Liu, Shelley D. Minteer, Nathan R. Neale, David Robertson, Adam P. Tornheim, Stephen E. Trask, Gabriel M. Veith, Ankit Verma, Zhenzhen YangChristopher Johnson

Research output: Contribution to journalArticlepeer-review

29 Scopus citations

Abstract

Li-ion batteries will lose both capacity and power over time due to calendar aging caused by slow parasitic processes that consume Li+ ions. Studying and mitigating these processes is traditionally an equally slow venture, which is especially taxing for the validation of new active materials and electrolyte additives. Here, we evaluate whether potentiostatic holds can be used to accelerate the diagnosis of Li+ loss during calendar aging. The technique is based on the idea that, under the right conditions, the current measured as the cell voltage is held constant can be correlated with the instantaneous rate of side reactions. Thus, in principle, these measurements could capture the rate of capacity fade in real time. In practice, we show that this method is incapable of quantitatively forecasting calendar aging trends. Instead, our study demonstrates that potentiostatic holds can be applied for initial qualitative screening of systems that exhibit promising long-term stability, which can be useful to shrink the parameter space for calendar aging studies. By facilitating the identification of improved formulations, this approach can help accelerate innovation in the battery industry.

Original languageEnglish
Article number050531
JournalJournal of the Electrochemical Society
Volume169
Issue number5
DOIs
StatePublished - May 2022

Funding

This research was supported by the U.S. Department of Energy’s Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham, and managed by Anthony Burrell. This work was conducted in part by the Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02–06CH11357. This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05–00OR22725 with the U.S. Department of Energy. Sandia National Laboratories is a multimission Laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. Lawrence Berkeley National Laboratory is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02–05CH11231. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes.

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