Lithium inventory tracking as a non-destructive battery evaluation and monitoring method

Li, Meng; Zhang, Yulun; Zhou, Hui; Xin, Fengxia; Whittingham, M. Stanley; Liaw, Boryann

doi:10.1038/s41560-024-01476-z

Title: Lithium inventory tracking as a non-destructive battery evaluation and monitoring method

Journal Article · 29 March 2024 · Nature Energy

DOI: https://doi.org/10.1038/s41560-024-01476-z · OSTI ID:2434007

^[1];

^[2];

^[1]

Idaho National Laboratory (INL), Idaho Falls, ID (United States)
State Univ. of New York (SUNY), Binghamton, NY (United States)

Tracking the active lithium (Li) inventory in an electrode shows the true state of a Li battery, akin to a fuel gauge for an engine. However, non-destructive Li inventory tracking is currently unavailable. Here, in this work, we used the theoretical capacity of a transition metal oxide to convert capacity into a Li inventory analysis. The Li inventory in electrodes was tracked reliably to show how battery formulations and test methods affect performance. Contrary to capacity, Li inventory tracking reveals stoichiometric variations near the electrode–electrolyte interface. Verifiable results rationalized differences in measurements, clarifying and reducing interferences from cell formulations and experimental manipulations. By tracing four variables from formation to end-of-life, we characterize electrode and cell performance with a thermodynamic framework. Accurate rationalization of subtle differences in Li inventory utilization promises precise battery engineering, evaluation, failure analysis and risk mitigation. The method could be applicable from cell design optimization and fabrication to battery management, improving battery performance and reliability.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2434007

Report Number(s):: INL/JOU--22-67897-Rev001

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 5 Vol. 9; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (35)

High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material Mao, Yuwei; Wang, Xuelong; Xia, Sihao Advanced Functional Materials, Vol. 29, Issue 18 https://doi.org/10.1002/adfm.201900247	journal	March 2019
Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries Adams, Brian D.; Zheng, Jianming; Ren, Xiaodi Advanced Energy Materials, Vol. 8, Issue 7 https://doi.org/10.1002/aenm.201702097	journal	October 2017
Origins and accommodation of cell variations in Li-ion battery pack modeling Dubarry, Matthieu; Vuillaume, Nicolas; Liaw, Bor Yann International Journal of Energy Research, Vol. 34, Issue 2 https://doi.org/10.1002/er.1668	journal	December 2009
Investigating the first-cycle irreversibility of lithium metal oxide cathodes for Li batteries Kang, Sun-Ho; Yoon, Won-Sub; Nam, Kyung-Wan Journal of Materials Science, Vol. 43, Issue 14 https://doi.org/10.1007/s10853-007-2355-6	journal	July 2008
Reversibility of LiNiO2 cathode Arai, H. Solid State Ionics, Vol. 95, Issue 3-4 https://doi.org/10.1016/S0167-2738(96)00598-X	journal	March 1997
Capacity loss in rechargeable lithium cells during cycle life testing: The importance of determining state-of-charge Dubarry, Matthieu; Svoboda, Vojtech; Hwu, Ruey Journal of Power Sources, Vol. 174, Issue 2 https://doi.org/10.1016/j.jpowsour.2007.06.185	journal	December 2007
Investigation of path dependence in commercial lithium-ion cells chosen for plug-in hybrid vehicle duty cycle protocols Gering, Kevin L.; Sazhin, Sergiy V.; Jamison, David K. Journal of Power Sources, Vol. 196, Issue 7 https://doi.org/10.1016/j.jpowsour.2010.05.058	journal	April 2011
Evaluation of commercial lithium-ion cells based on composite positive electrode for plug-in hybrid electric vehicle applications. Part I: Initial characterizations Dubarry, Matthieu; Truchot, Cyril; Cugnet, Mikaël Journal of Power Sources, Vol. 196, Issue 23 https://doi.org/10.1016/j.jpowsour.2011.08.077	journal	December 2011
Path dependence of lithium ion cells aging under storage conditions Su, Laisuo; Zhang, Jianbo; Huang, Jun Journal of Power Sources, Vol. 315 https://doi.org/10.1016/j.jpowsour.2016.03.043	journal	May 2016
On state-of-charge determination for lithium-ion batteries Li, Zhe; Huang, Jun; Liaw, Bor Yann Journal of Power Sources, Vol. 348 https://doi.org/10.1016/j.jpowsour.2017.03.001	journal	April 2017
Review on comprehending and enhancing the initial Coulombic efficiency of anode materials in lithium-ion/sodium-ion batteries Li, Xin; Sun, Xiaohong; Hu, Xudong Nano Energy, Vol. 77 https://doi.org/10.1016/j.nanoen.2020.105143	journal	November 2020
Synchrotron Operando Depth Profiling Studies of State-of-Charge Gradients in Thick Li(Ni _0.8 Mn _0.1 Co _0.1 )O ₂ Cathode Films Li, Zhuo; Yin, Liang; Mattei, Gerard S. Chemistry of Materials, Vol. 32, Issue 15 https://doi.org/10.1021/acs.chemmater.0c00983	journal	July 2020
Evolution of Structure and Lithium Dynamics in LiNi _0.8 Mn _0.1 Co _0.1 O ₂ (NMC811) Cathodes during Electrochemical Cycling Märker, Katharina; Reeves, Philip J.; Xu, Chao Chemistry of Materials, Vol. 31, Issue 7 https://doi.org/10.1021/acs.chemmater.9b00140	journal	March 2019
Li–Nb–O Coating/Substitution Enhances the Electrochemical Performance of the LiNi _0.8 Mn _0.1 Co _0.1 O ₂ (NMC 811) Cathode Xin, Fengxia; Zhou, Hui; Chen, Xiaobo ACS Applied Materials & Interfaces, Vol. 11, Issue 38 https://doi.org/10.1021/acsami.9b09696	journal	June 2019
What Limits the Capacity of Layered Oxide Cathodes in Lithium Batteries? Zhou, Hui; Xin, Fengxia; Pei, Ben ACS Energy Letters, Vol. 4, Issue 8 https://doi.org/10.1021/acsenergylett.9b01236	journal	July 2019
Formation of Surface Impurities on Lithium–Nickel–Manganese–Cobalt Oxides in the Presence of CO₂ and H₂O Fang, Zongtang; Confer, Matthew P.; Wang, Yixiao Journal of the American Chemical Society, Vol. 143, Issue 27 https://doi.org/10.1021/jacs.1c03812	journal	July 2021
Combined operando X-ray diffraction–electrochemical impedance spectroscopy detecting solid solution reactions of LiFePO4 in batteries Hess, Michael; Sasaki, Tsuyoshi; Villevieille, Claire Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9169	journal	September 2015
Pathways for practical high-energy long-cycling lithium metal batteries Liu, Jun; Bao, Zhenan; Cui, Yi Nature Energy, Vol. 4, Issue 3 https://doi.org/10.1038/s41560-019-0338-x	journal	February 2019
Understanding and applying coulombic efficiency in lithium metal batteries Xiao, Jie; Li, Qiuyan; Bi, Yujing Nature Energy, Vol. 5, Issue 8 https://doi.org/10.1038/s41560-020-0648-z	journal	June 2020
Effects of cycling on lithium-ion battery hysteresis and overvoltage Ovejas, V. J.; Cuadras, A. Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-51474-5	journal	October 2019
The truth about the 1st cycle Coulombic efficiency of LiNi _1/3 Co _1/3 Mn _1/3 O ₂ (NCM) cathodes Kasnatscheew, J.; Evertz, M.; Streipert, B. Physical Chemistry Chemical Physics, Vol. 18, Issue 5 https://doi.org/10.1039/C5CP07718D	journal	January 2016
Cell degradation quantification—a performance metric-based approach Zhang, Yulun; Wang, Qiang; Liaw, Boryann Journal of Physics: Energy, Vol. 2, Issue 3 https://doi.org/10.1088/2515-7655/ab979b	journal	July 2020
Modeling and analysis of battery hysteresis effects Rahimi Eichi, Habiballah; Chow, Mo-Yuen 2012 IEEE Energy Conversion Congress and Exposition (ECCE) https://doi.org/10.1109/ECCE.2012.6342212	conference	September 2012
Origin and hysteresis of lithium compositional spatiodynamics within battery primary particles Lim, Jongwoo; Li, Yiyang; Alsem, Daan Hein Science, Vol. 353, Issue 6299 https://doi.org/10.1126/science.aaf4914	journal	August 2016
Electrochemical and Structural Characterization of LiNi[sub 1−y]Co[sub y]O[sub 2] (0 ≤ y ≤ 0.2) Positive Electrodes during Initial Cycling Lee, Kyung-Keun; Kim, Kwang-Bum Journal of The Electrochemical Society, Vol. 147, Issue 5 https://doi.org/10.1149/1.1393422	journal	January 2000
Formation of Solid Electrolyte Interface in Lithium Nickel Mixed Oxide Electrodes during the First Cycling Zhang, S. S.; Xu, K.; Jow, T. R. Electrochemical and Solid-State Letters, Vol. 5, Issue 5 https://doi.org/10.1149/1.1464506	journal	January 2002
Investigation of the Irreversible Capacity Loss in the Layered LiNi[sub 1∕3]Mn[sub 1∕3]Co[sub 1∕3]O[sub 2] Cathodes Choi, J.; Manthiram, A. Electrochemical and Solid-State Letters, Vol. 8, Issue 8 https://doi.org/10.1149/1.1943567	journal	January 2005
Determination of the Kinetic Parameters of Mixed-Conducting Electrodes and Application to the System Li[sub 3]Sb Weppner, W. Journal of The Electrochemical Society, Vol. 124, Issue 10 https://doi.org/10.1149/1.2133112	journal	January 1977
Precision Measurements of the Coulombic Efficiency of Lithium-Ion Batteries and of Electrode Materials for Lithium-Ion Batteries Smith, A. J.; Burns, J. C.; Trussler, S. Journal of The Electrochemical Society, Vol. 157, Issue 2 https://doi.org/10.1149/1.3268129	journal	January 2010
A Quantitative Failure Analysis on Capacity Fade in Rechargeable Lithium Metal Cells Zhang, Yulun; Wang, Qiang; Liaw, Boryann Journal of The Electrochemical Society, Vol. 167, Issue 9 https://doi.org/10.1149/1945-7111/ab6cf4	journal	January 2020
Does Polarization Increase Lead to Capacity Fade? Wang, Fuqing; Lin, Zhen; Liu, Lijuan Journal of The Electrochemical Society, Vol. 167, Issue 9 https://doi.org/10.1149/1945-7111/ab956b	journal	June 2020
What do Coulombic Efficiency and Capacity Retention Truly Measure? A Deep Dive into Cyclable Lithium Inventory, Limitation Type, and Redox Side Reactions Tornheim, Adam; O’Hanlon, Daniel C. Journal of The Electrochemical Society, Vol. 167, Issue 11 https://doi.org/10.1149/1945-7111/ab9ee8	journal	July 2020
Improving Precision and Accuracy in Coulombic Efficiency Measurements of Li-Ion Batteries Bond, T. M.; Burns, J. C.; Stevens, D. A. Journal of The Electrochemical Society, Vol. 160, Issue 3 https://doi.org/10.1149/2.014304jes	journal	January 2013
Understanding Anomalous Behavior in Coulombic Efficiency Measurements on Li-Ion Batteries Gyenes, Balazs; Stevens, D. A.; Chevrier, V. L. Journal of The Electrochemical Society, Vol. 162, Issue 3 https://doi.org/10.1149/2.0191503jes	journal	December 2014
Removing the Intrinsic NiO Phase and Residual Lithium for High-Performance Nickel-Rich Materials Wu, Feng; Dong, Jinyang; Chen, Lai Energy Material Advances, Vol. 4 https://doi.org/10.34133/energymatadv.0007	journal	January 2023

Similar Records

Probing lithiation and delithiation of thick sintered lithium-ion battery electrodes with neutron imaging

Journal Article · 2019 · Journal of Power Sources · OSTI ID:1526376

Nie, Ziyang; McCormack, Patrick; Bilheux, Hassina Z.; +4 more

Capacity fade in high energy silicon-graphite electrodes for lithium-ion batteries

Journal Article · 2018 · ChemComm · OSTI ID:1439867

Dose, W. M.; Piernas-Munoz, M. J.; Maroni, V. A.; +3 more

Conformal Pressure and Fast-Charging Li-Ion Batteries

Journal Article · 2022 · Journal of the Electrochemical Society · OSTI ID:1863095

Cao, Chuntian; Steinrück, Hans-Georg; Paul, Partha P.; +13 more

Related Subjects

25 ENERGY STORAGE
36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
42 ENGINEERING
Li content in cathode
Li inventory tracking
cathode utilization efficiency and coefficient
electrochemical analytic diagnosis
rechargeable Li batteries

Title: Lithium inventory tracking as a non-destructive battery evaluation and monitoring method

Citation Formats

References (35)

Similar Records

Related Subjects