Structural Evolution and Transition Dynamics in Lithium Ion Battery under Fast Charging: An Operando Neutron Diffraction Investigation

Wu, Xianyang; Song, Bohang; Chien, Po‐Hsiu; Everett, S. Michelle; Zhao, Kejie; Liu, Jue; Du, Zhijia

doi:10.1002/advs.202102318

Title: Structural Evolution and Transition Dynamics in Lithium Ion Battery under Fast Charging: An Operando Neutron Diffraction Investigation

Journal Article · 08 September 2021 · Advanced Science

DOI: https://doi.org/10.1002/advs.202102318 · OSTI ID:1819232

Wu, Xianyang ^[1]; Song, Bohang ^[2]; Chien, Po‐Hsiu ^[2]; Everett, S. Michelle ^[2]; Zhao, Kejie ^[3]; Liu, Jue ^[2];

^[4]

Electrification and Energy Infrastructures Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA, School of Mechanical Engineering Purdue University West Lafayette IN 47907 USA, Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA
Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA
School of Mechanical Engineering Purdue University West Lafayette IN 47907 USA
Electrification and Energy Infrastructures Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA

Abstract Fast charging (<15 min) of lithium‐ion batteries (LIBs) for electrical vehicles (EVs) is widely seen as the key factor that will greatly stimulate the EV markets, and its realization is mainly hindered by the sluggish diffusion of Li ⁺ . To have a mechanistic understanding of Li ⁺ diffusion within LIBs, in this study, structural evolutions of electrodes for a Ni‐rich LiNi _0.6 Mn _0.2 Co _0.2 O ₂ (NMC622) || graphite cylindrical cell with high areal loading (2.78 mAh cm ⁻² ) are developed for operando neutron powder diffraction study at different charging rates. Via sequential Rietveld refinements, changes in structures of NMC622 and Li _x C ₆ are obtained during moderate and fast charging (from 0.27 C to 4.4 C). NMC622 exhibits the same structural evolution regardless of C‐rates. For phase transitions of Li _x C ₆ , the stage I (LiC ₆ ) phase emerges earlier during the stepwise intercalation at a lower state of charge when charging rate is increased. It is also found that the stage II (LiC ₁₂ ) → stage I (LiC ₆ ) transition is the rate‐limiting step during fast charging. The LiC ₁₂ → LiC ₆ transition mechanism is further analyzed using the Johnson–Mehl–Avrami–Kolmogorov model. It is concluded as a diffusion‐controlled, 1D phase transition with decreasing nucleation kinetics under increasing chargingrates.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1819232

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 21 Vol. 8; ISSN 2198-3844

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Dependence of Cell Failure on Cut-Off Voltage Ranges and Observation of Kinetic Hindrance in LiNi _0.8 Co _0.15 Al _0.05 O ₂ Li, Jing; Harlow, Jessie; Stakheiko, Nikolai Journal of The Electrochemical Society, Vol. 165, Issue 11 https://doi.org/10.1149/2.0491811jes	journal	January 2018
High Rate Capability of Li(Ni _1/3 Mn _1/3 Co _1/3 )O ₂ Electrode for Li-Ion Batteries Wu, Shao-Ling; Zhang, Wei; Song, Xiangyun Journal of The Electrochemical Society, Vol. 159, Issue 4 https://doi.org/10.1149/2.062204jes	journal	January 2012
A New Null Matrix Electrochemical Cell for Rietveld Refinements of In-Situ or Operando Neutron Powder Diffraction Data Bianchini, M.; Leriche, J. B.; Laborier, J. -L. Journal of The Electrochemical Society, Vol. 160, Issue 11 https://doi.org/10.1149/2.076311jes	journal	January 2013
An In-Situ Electrochemical Cell for Neutron Diffraction Studies of Phase Transitions in Small Volume Electrodes of Li-Ion Batteries Vadlamani, B.; An, K.; Jagannathan, M. Journal of The Electrochemical Society, Vol. 161, Issue 10 https://doi.org/10.1149/2.0951410jes	journal	January 2014
Depth-Dependent Redox Behavior of LiNi _0.6 Mn _0.2 Co _0.2 O ₂ Tian, Chixia; Nordlund, Dennis; Xin, Huolin L. Journal of The Electrochemical Society, Vol. 165, Issue 3 https://doi.org/10.1149/2.1021803jes	journal	January 2018
In Situ Neutron Diffraction Study of Lithiation Gradients in Graphite Anodes during Discharge and Relaxation Wilhelm, Jörn; Seidlmayer, Stefan; Erhard, Simon Journal of The Electrochemical Society, Vol. 165, Issue 9 https://doi.org/10.1149/2.1231809jes	journal	January 2018
An Analytical Method to Determine Tortuosity in Rechargeable Battery Electrodes Vijayaraghavan, Bharath; Ely, David R.; Chiang, Yet-Ming Journal of The Electrochemical Society, Vol. 159, Issue 5 https://doi.org/10.1149/2.jes113224	journal	January 2012
In situ analysis of LiFePO ₄ batteries: Signal extraction by multivariate analysis Rodriguez, Mark A.; Van Benthem, Mark H.; Ingersoll, David Powder Diffraction, Vol. 25, Issue 2 https://doi.org/10.1154/1.3393786	journal	June 2010
Use of electrochemical methods to determine chemical-diffusion coefficients in alloys: application to ‘LiAI’ Wen, C. J.; Ho, C.; Boukamp, B. A. International Materials Reviews, Vol. 26, Issue 1 https://doi.org/10.1179/imr.1981.26.1.253	journal	January 1981
Diffusive Motion in Stage-1 and Stage-2 Li-Graphite Intercalation Compounds: Results of ß-NMR and Quasielastic Neutron Scattering Schirmer, A.; Heitjans, P. Zeitschrift für Naturforschung A, Vol. 50, Issue 7 https://doi.org/10.1515/zna-1995-0704	journal	July 1995
A Cylindrical Cell for Operando Neutron Diffraction of Li-Ion Battery Electrode Materials Vitoux, Laura; Reichardt, Martin; Sallard, Sébastien Frontiers in Energy Research, Vol. 6 https://doi.org/10.3389/fenrg.2018.00076	journal	August 2018

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