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

Nie, Ziyang; McCormack, Patrick; Bilheux, Hassina Z.; Bilheux, Jean Christophe; Robinson, J. Pierce; Nanda, Jagjit; Koenig, Jr., Gary M.

doi:10.1016/j.jpowsour.2019.02.075

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

Journal Article · Fri Mar 01 00:00:00 EST 2019 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2019.02.075· OSTI ID:1526376

Nie, Ziyang ^[1]; McCormack, Patrick ^[1];

^[2];

^[2]; Robinson, J. Pierce ^[1];

^[2];

^[1]

Univ. of Virginia, Charlottesville, VA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

As lithium-on (Li-ion) batteries increase in their prevalence and the range of applications expands, there is a need to understand and exploit the limits of electrochemical performance. Probing the internal processes in Li-ion batteries provides insights into the electrochemical characteristics of the cells as well as information necessary for rational cell design. In this manuscript an in situ method, neutron imaging, is applied to Li-ion full cells to track the lithiation/delithiation processes in the electrodes during discharge. The electrodes comprise thick sintered films of only active material, which improves the number of discrete points that are mapped for net changes in neutron intensity through the electrode. The lithiation/delithiation processes are qualitatively consistent with calculations of the Li⁺ concentration and discharge profiles of the cells. These results illustrate that neutron imaging can experimentally probe and confirm limitations in the electrochemical performance of Li-ion full cells, particularly those with thick electrodes.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1526376

Alternate ID(s):: OSTI ID: 1636520

Journal Information:: Journal of Power Sources, Vol. 419, Issue C; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 26 works

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References (41)

Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
Lithium and Lithium-Ion Batteries: Challenges and Prospects Passerini, S.; Scrosati, B. Interface magazine, Vol. 25, Issue 3 https://doi.org/10.1149/2.F09163if	journal	January 2016
In Situ Observation of the Electrochemical Lithiation of a Single SnO₂ Nanowire Electrode Huang, J. Y.; Zhong, L.; Wang, C. M. Science, Vol. 330, Issue 6010, p. 1515-1520 https://doi.org/10.1126/science.1195628	journal	December 2010
Electrochemical and In Situ X‐Ray Diffraction Studies of Lithium Intercalation in Li_xCoO₂ Reimers, Jan N.; Dahn, J. R. Journal of The Electrochemical Society, Vol. 139, Issue 8, p. 2091-2097 https://doi.org/10.1149/1.2221184	journal	January 1992
Optimizing Areal Capacities through Understanding the Limitations of Lithium-Ion Electrodes Gallagher, Kevin G.; Trask, Stephen E.; Bauer, Christoph Journal of The Electrochemical Society, Vol. 163, Issue 2 https://doi.org/10.1149/2.0321602jes	journal	November 2015
Quantitative Visualization of Salt Concentration Distributions in Lithium-Ion Battery Electrolytes during Battery Operation Using X-ray Phase Imaging Takamatsu, Daiko; Yoneyama, Akio; Asari, Yusuke Journal of the American Chemical Society, Vol. 140, Issue 5 https://doi.org/10.1021/jacs.7b13357	journal	January 2018
In Situ Three-Dimensional Synchrotron X-Ray Nanotomography of the (De)lithiation Processes in Tin Anodes Wang, Jiajun; Chen-Wiegart, Yu-chen Karen; Wang, Jun Angewandte Chemie International Edition, Vol. 53, Issue 17 https://doi.org/10.1002/anie.201310402	journal	March 2014
Probing Multiscale Transport and Inhomogeneity in a Lithium-Ion Pouch Cell Using In Situ Neutron Methods Zhou, Hui; An, Ke; Allu, Srikanth ACS Energy Letters, Vol. 1, Issue 5 https://doi.org/10.1021/acsenergylett.6b00353	journal	October 2016
Neutron Imaging of Lithium Concentration in LFP Pouch Cell Battery Siegel, Jason B.; Lin, Xinfan; Stefanopoulou, Anna G. Journal of The Electrochemical Society, Vol. 158, Issue 5 https://doi.org/10.1149/1.3566341	journal	January 2011
Imaging of the Li spatial distribution within V2O5 cathode in a coin cell by neutron computed tomography Zhang, Yuxuan; Chandran, K. S. Ravi; Bilheux, Hassina Z. Journal of Power Sources, Vol. 376 https://doi.org/10.1016/j.jpowsour.2017.11.080	journal	February 2018
Thick Electrodes for High Energy Lithium Ion Batteries Singh, Madhav; Kaiser, Jörg; Hahn, Horst Journal of The Electrochemical Society, Vol. 162, Issue 7 https://doi.org/10.1149/2.0401507jes	journal	January 2015
Sintered electrode full cells for high energy density lithium-ion batteries Robinson, J. Pierce; Ruppert, John J.; Dong, Hongxu Journal of Applied Electrochemistry, Vol. 48, Issue 11 https://doi.org/10.1007/s10800-018-1242-y	journal	August 2018
Ultrahigh-Energy-Density Microbatteries Enabled by New Electrode Architecture and Micropackaging Design Lai, Wei; Erdonmez, Can K.; Marinis, Thomas F. Advanced Materials, Vol. 22, Issue 20 https://doi.org/10.1002/adma.200903650	journal	May 2010
Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell Doyle, Marc Journal of The Electrochemical Society, Vol. 140, Issue 6 https://doi.org/10.1149/1.2221597	journal	January 1993
Simulation and Optimization of the Dual Lithium Ion Insertion Cell Fuller, Thomas F. Journal of The Electrochemical Society, Vol. 141, Issue 1 https://doi.org/10.1149/1.2054684	journal	January 1994
Relaxation Phenomena in Lithium-Ion-Insertion Cells Fuller, Thomas F. Journal of The Electrochemical Society, Vol. 141, Issue 4 https://doi.org/10.1149/1.2054868	journal	January 1994
High-Performance LiCoO ₂ Sub-Micrometer Materials from Scalable Microparticle Template Processing Qi, Zhaoxiang; Koenig, Gary M. ChemistrySelect, Vol. 1, Issue 13 https://doi.org/10.1002/slct.201600872	journal	August 2016
A carbon-free lithium-ion solid dispersion redox couple with low viscosity for redox flow batteries Qi, Zhaoxiang; Koenig, Gary M. Journal of Power Sources, Vol. 323 https://doi.org/10.1016/j.jpowsour.2016.05.033	journal	August 2016
The CG-1D Neutron Imaging Beamline at the Oak Ridge National Laboratory High Flux Isotope Reactor Santodonato, Lou; Bilheux, Hassina; Bailey, Barton Physics Procedia, Vol. 69 https://doi.org/10.1016/j.phpro.2015.07.015	journal	January 2015
Determination of chromium and cobalt in human serum by neutron activation analysis. Versieck, J.; Hoste, J.; Barbier, F. Clinical Chemistry, Vol. 24, Issue 2 https://doi.org/10.1093/clinchem/24.2.303	journal	February 1978
A new open computational framework for highly-resolved coupled three-dimensional multiphysics simulations of Li-ion cells Allu, Srikanth; Kalnaus, Sergiy; Elwasif, Wael Journal of Power Sources, Vol. 246 https://doi.org/10.1016/j.jpowsour.2013.08.040	journal	January 2014
Li-ion battery materials: present and future Nitta, Naoki; Wu, Feixiang; Lee, Jung Tae Materials Today, Vol. 18, Issue 5 https://doi.org/10.1016/j.mattod.2014.10.040	journal	June 2015
A comparative study of Li-ion battery, supercapacitor and nonaqueous asymmetric hybrid devices for automotive applications Du Pasquier, Aurelien; Plitz, Irene; Menocal, Serafin Journal of Power Sources, Vol. 115, Issue 1, p. 171-178 https://doi.org/10.1016/S0378-7753(02)00718-8	journal	March 2003
A comprehensive understanding of electrode thickness effects on the electrochemical performances of Li-ion battery cathodes Zheng, Honghe; Li, Jing; Song, Xiangyun Electrochimica Acta, Vol. 71, p. 258-265 https://doi.org/10.1016/j.electacta.2012.03.161	journal	June 2012
State of the art of commercial Li ion batteries Moshtev, R.; Johnson, B. Journal of Power Sources, Vol. 91, Issue 2 https://doi.org/10.1016/S0378-7753(00)00458-4	journal	December 2000
Numerical modelling of transport limitations in lithium titanate anodes Rashid, Muhammad; Sahoo, Asit; Gupta, Amit Electrochimica Acta, Vol. 283 https://doi.org/10.1016/j.electacta.2018.06.147	journal	September 2018
The insulator-metal transition upon lithium deintercalation from LiCoO2: electronic properties and 7Li NMR study Ménétrier, Michel; Saadoune, Ismael; Levasseur, Stéphane Journal of Materials Chemistry, Vol. 9, Issue 5 https://doi.org/10.1039/a900016j	journal	January 1999
Electronic Conductivity in the Li _4/3 Ti _5/3 O ₄ -Li _7/3 Ti _5/3 O ₄ System and Variation with State-of-Charge as a Li Battery Anode Young, David; Ransil, Alan; Amin, Ruhul Advanced Energy Materials, Vol. 3, Issue 9 https://doi.org/10.1002/aenm.201300134	journal	April 2013
Electrochemical study of Li4Ti5O12 as negative electrode for Li-ion polymer rechargeable batteries Zaghib, K.; Simoneau, M.; Armand, M. Journal of Power Sources, Vol. 81-82 https://doi.org/10.1016/S0378-7753(99)00209-8	journal	September 1999
Electrochemical characterization of lithium cobalt oxide within aqueous flow suspensions as an indicator of rate capability in lithium-ion battery electrodes Geng, Linxiao; Denecke, Matthew E.; Foley, Sonia B. Electrochimica Acta, Vol. 281 https://doi.org/10.1016/j.electacta.2018.06.037	journal	August 2018
Single crystal growth and structure refinement of Li4Ti5O12 Kataoka, Kunimitsu; Takahashi, Yasuhiko; Kijima, Norihito Journal of Physics and Chemistry of Solids, Vol. 69, Issue 5-6 https://doi.org/10.1016/j.jpcs.2007.10.134	journal	May 2008
Structure and electron density analysis of electrochemically and chemically delithiated LiCoO₂ single crystals Takahashi, Yasuhiko; Kijima, Norihito; Dokko, Kaoru Journal of Solid State Chemistry, Vol. 180, Issue 1, p. 313-321 https://doi.org/10.1016/j.jssc.2006.10.018	journal	January 2007
Spherical Li4Ti5O12 synthesized by spray drying from a different kind of solution He, Zhenjiang; Wang, Zhixing; Wu, Feixiang Journal of Alloys and Compounds, Vol. 540 https://doi.org/10.1016/j.jallcom.2012.06.044	journal	November 2012
Semi-empirical modeling of charge and discharge profiles for a LiCoO2 electrode Zhang, Qi; Guo, Qingzhi; White, Ralph E. Journal of Power Sources, Vol. 165, Issue 1 https://doi.org/10.1016/j.jpowsour.2006.12.025	journal	February 2007
A review of conduction phenomena in Li-ion batteries Park, Myounggu; Zhang, Xiangchun; Chung, Myoungdo Journal of Power Sources, Vol. 195, Issue 24 https://doi.org/10.1016/j.jpowsour.2010.06.060	journal	December 2010
Anomalous Discharge Product Distribution in Lithium-Air Cathodes Nanda, Jagjit; Bilheux, Hassina; Voisin, Sophie The Journal of Physical Chemistry C, Vol. 116, Issue 15 https://doi.org/10.1021/jp3016003	journal	April 2012
Influence of the Binder on Lithium Ion Battery Electrode Tortuosity and Performance Landesfeind, Johannes; Eldiven, Askin; Gasteiger, Hubert A. Journal of The Electrochemical Society, Vol. 165, Issue 5 https://doi.org/10.1149/2.0971805jes	journal	January 2018
Unveiling the Roles of Binder in the Mechanical Integrity of Electrodes for Lithium-Ion Batteries Chen, Jianchao; Liu, Jianyong; Qi, Yue Journal of The Electrochemical Society, Vol. 160, Issue 9 https://doi.org/10.1149/2.088309jes	journal	January 2013
Tortuosity of Binder-Free and Carbon-Free High Energy Density LiCoO2 Electrodes for Rechargeable Lithium-Ion Batteries Cobb, C. L.; Bae, C. -J. ECS Transactions, Vol. 58, Issue 13 https://doi.org/10.1149/05813.0013ecst	journal	February 2014
Quantifying tortuosity in porous Li-ion battery materials Thorat, Indrajeet V.; Stephenson, David E.; Zacharias, Nathan A. Journal of Power Sources, Vol. 188, Issue 2 https://doi.org/10.1016/j.jpowsour.2008.12.032	journal	March 2009
Simplified calculation of the area specific impedance for battery design Gallagher, Kevin G.; Nelson, Paul A.; Dees, Dennis W. Journal of Power Sources, Vol. 196, Issue 4 https://doi.org/10.1016/j.jpowsour.2010.10.020	journal	February 2011

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