Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging

Jiyu Cai; Xinwei Zhou; Tianyi Li; Hoai T. Nguyen; Gabriel M. Veith; Yan Qin; Wenquan Lu; Stephen E. Trask; Marco Tulio Fonseca Rodrigues; Yuzi Liu; Wenqian Xu; Maxwell C. Schulze; Anthony K. Burrell; Zonghai Chen

doi:10.1021/acsami.3c08015

Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging

Jiyu Cai, Xinwei Zhou, Tianyi Li, Hoai T. Nguyen, Gabriel M. Veith, Yan Qin, Wenquan Lu, Stephen E. Trask, Marco Tulio Fonseca Rodrigues, Yuzi Liu, Wenqian Xu, Maxwell C. Schulze, Anthony K. Burrell, Zonghai Chen

Energy Storage & Conversion

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Increasing the energy density of lithium-ion batteries, and thereby reducing costs, is a major target for industry and academic research. One of the best opportunities is to replace the traditional graphite anode with a high-capacity anode material, such as silicon. However, Si-based lithium-ion batteries have been widely reported to suffer from a limited calendar life for automobile applications. Heretofore, there lacks a fundamental understanding of calendar aging for rationally developing mitigation strategies. Both open-circuit voltage and voltage-hold aging protocols were utilized to characterize the aging behavior of Si-based cells. Particularly, a high-precision leakage current measurement was applied to quantitatively measure the rate of parasitic reactions at the electrode/electrolyte interface. The rate of parasitic reactions at the Si anode was found 5 times and 15 times faster than those of LiNi_0.8Mn_0.1Co_0.1O₂ and LiFePO₄ cathodes, respectively. The imbalanced charge loss from parasitic reactions plays a critical role in exacerbating performance deterioration. In addition, a linear relationship between capacity loss and charge consumption from parasitic reactions provides fundamental support to assess calendar life through voltage-hold tests. These new findings imply that longer calendar life can be achieved by suppressing parasitic reactions at the Si anode to balance charge consumption during calendar aging.

Original language	English
Pages (from-to)	48085-48095
Number of pages	11
Journal	ACS Applied Materials and Interfaces
Volume	15
Issue number	41
DOIs	https://doi.org/10.1021/acsami.3c08015
State	Published - Oct 18 2023

Funding

Research at Argonne National Laboratory was supported by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office under the Silicon Consortium Seedling project (VT1201000-05450-1005554). Argonne National Laboratory is operated for the DOE Office of Science by UChicago Argonne, LLC, under Contract DE-AC02-06CH11357. Materials development 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. The authors also acknowledge the use of the Advanced Photon Source (APS) and the Center for Nanoscale Materials (CNM) that are supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. The authors also acknowledge great support and input from the National Renewable Energy Laboratory (NREL), operated by Alliance for Sustainable Energy, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. A portion of this manuscript (GMV) has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy. The authors also acknowledge the valuable discussion with team members of the Silicon Consortium Project.

Keywords

Si anode
calendar aging
charge balance
parasitic reactions
steady leakage current

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10.1021/acsami.3c08015

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Cai, J., Zhou, X., Li, T., Nguyen, H. T., Veith, G. M., Qin, Y., Lu, W., Trask, S. E., Fonseca Rodrigues, M. T., Liu, Y., Xu, W., Schulze, M. C., Burrell, A. K., & Chen, Z. (2023). Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging. ACS Applied Materials and Interfaces, 15(41), 48085-48095. https://doi.org/10.1021/acsami.3c08015

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title = "Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging",

abstract = "Increasing the energy density of lithium-ion batteries, and thereby reducing costs, is a major target for industry and academic research. One of the best opportunities is to replace the traditional graphite anode with a high-capacity anode material, such as silicon. However, Si-based lithium-ion batteries have been widely reported to suffer from a limited calendar life for automobile applications. Heretofore, there lacks a fundamental understanding of calendar aging for rationally developing mitigation strategies. Both open-circuit voltage and voltage-hold aging protocols were utilized to characterize the aging behavior of Si-based cells. Particularly, a high-precision leakage current measurement was applied to quantitatively measure the rate of parasitic reactions at the electrode/electrolyte interface. The rate of parasitic reactions at the Si anode was found 5 times and 15 times faster than those of LiNi0.8Mn0.1Co0.1O2 and LiFePO4 cathodes, respectively. The imbalanced charge loss from parasitic reactions plays a critical role in exacerbating performance deterioration. In addition, a linear relationship between capacity loss and charge consumption from parasitic reactions provides fundamental support to assess calendar life through voltage-hold tests. These new findings imply that longer calendar life can be achieved by suppressing parasitic reactions at the Si anode to balance charge consumption during calendar aging.",

keywords = "Si anode, calendar aging, charge balance, parasitic reactions, steady leakage current",

author = "Jiyu Cai and Xinwei Zhou and Tianyi Li and Nguyen, \{Hoai T.\} and Veith, \{Gabriel M.\} and Yan Qin and Wenquan Lu and Trask, \{Stephen E.\} and \{Fonseca Rodrigues\}, \{Marco Tulio\} and Yuzi Liu and Wenqian Xu and Schulze, \{Maxwell C.\} and Burrell, \{Anthony K.\} and Zonghai Chen",

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Cai, J, Zhou, X, Li, T, Nguyen, HT, Veith, GM, Qin, Y, Lu, W, Trask, SE, Fonseca Rodrigues, MT, Liu, Y, Xu, W, Schulze, MC, Burrell, AK & Chen, Z 2023, 'Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging', ACS Applied Materials and Interfaces, vol. 15, no. 41, pp. 48085-48095. https://doi.org/10.1021/acsami.3c08015

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T1 - Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging

AU - Cai, Jiyu

AU - Zhou, Xinwei

AU - Li, Tianyi

AU - Nguyen, Hoai T.

AU - Veith, Gabriel M.

AU - Qin, Yan

AU - Lu, Wenquan

AU - Trask, Stephen E.

AU - Fonseca Rodrigues, Marco Tulio

AU - Liu, Yuzi

AU - Xu, Wenqian

AU - Schulze, Maxwell C.

AU - Burrell, Anthony K.

AU - Chen, Zonghai

PY - 2023/10/18

Y1 - 2023/10/18

N2 - Increasing the energy density of lithium-ion batteries, and thereby reducing costs, is a major target for industry and academic research. One of the best opportunities is to replace the traditional graphite anode with a high-capacity anode material, such as silicon. However, Si-based lithium-ion batteries have been widely reported to suffer from a limited calendar life for automobile applications. Heretofore, there lacks a fundamental understanding of calendar aging for rationally developing mitigation strategies. Both open-circuit voltage and voltage-hold aging protocols were utilized to characterize the aging behavior of Si-based cells. Particularly, a high-precision leakage current measurement was applied to quantitatively measure the rate of parasitic reactions at the electrode/electrolyte interface. The rate of parasitic reactions at the Si anode was found 5 times and 15 times faster than those of LiNi0.8Mn0.1Co0.1O2 and LiFePO4 cathodes, respectively. The imbalanced charge loss from parasitic reactions plays a critical role in exacerbating performance deterioration. In addition, a linear relationship between capacity loss and charge consumption from parasitic reactions provides fundamental support to assess calendar life through voltage-hold tests. These new findings imply that longer calendar life can be achieved by suppressing parasitic reactions at the Si anode to balance charge consumption during calendar aging.

AB - Increasing the energy density of lithium-ion batteries, and thereby reducing costs, is a major target for industry and academic research. One of the best opportunities is to replace the traditional graphite anode with a high-capacity anode material, such as silicon. However, Si-based lithium-ion batteries have been widely reported to suffer from a limited calendar life for automobile applications. Heretofore, there lacks a fundamental understanding of calendar aging for rationally developing mitigation strategies. Both open-circuit voltage and voltage-hold aging protocols were utilized to characterize the aging behavior of Si-based cells. Particularly, a high-precision leakage current measurement was applied to quantitatively measure the rate of parasitic reactions at the electrode/electrolyte interface. The rate of parasitic reactions at the Si anode was found 5 times and 15 times faster than those of LiNi0.8Mn0.1Co0.1O2 and LiFePO4 cathodes, respectively. The imbalanced charge loss from parasitic reactions plays a critical role in exacerbating performance deterioration. In addition, a linear relationship between capacity loss and charge consumption from parasitic reactions provides fundamental support to assess calendar life through voltage-hold tests. These new findings imply that longer calendar life can be achieved by suppressing parasitic reactions at the Si anode to balance charge consumption during calendar aging.

KW - Si anode

KW - calendar aging

KW - charge balance

KW - parasitic reactions

KW - steady leakage current

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JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 41

ER -

Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging

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