Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes
Abstract
The performance of lithium ion electrodes is hindered by unfavorable chemical heterogeneities that pre-exist or develop during operation. Time-resolved spatial descriptions are needed to understand the link between such heterogeneities and a cell's performance. Here, operando high-resolution X-ray diffraction-computed tomography is used to spatially and temporally quantify crystallographic heterogeneities within and between particles throughout both fresh and degraded LixMn2O4 electrodes. This imaging technique facilitates identification of stoichiometric differences between particles and stoichiometric gradients and phase heterogeneities within particles. Through radial quantification of phase fractions, the response of distinct particles to lithiation is found to vary; most particles contain localized regions that transition to rock salt LiMnO2 within the first cycle. Other particles contain monoclinic Li2MnO3 near the surface and almost pure spinel LixMn2O4 near the core. Following 150 cycles, concentrations of LiMnO2 and Li2MnO3 significantly increase and widely vary between particles.
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- European Synchrotron Radiation Facility (ESRF), Grenoble (France); Finden Limited, Abingdon (United Kingdom); Univ. College London (United Kingdom)
- Univ. College London (United Kingdom); The Faraday Inst. (United Kingdom)
- Univ. College London (United Kingdom)
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
- European Synchrotron Radiation Facility (ESRF), Grenoble (France)
- Finden Limited, Abingdon (United Kingdom)
- Finden Limited, Abingdon (United Kingdom); Univ. College London (United Kingdom); Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Rutherford Appleton Lab. (RAL)
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); European Union Horizon 2020 Research and Innovation Program; Royal Academy of Engineering; The Faraday Institution
- OSTI Identifier:
- 1601577
- Report Number(s):
- NREL/JA-5400-75809
Journal ID: ISSN 2041-1723
- Grant/Contract Number:
- AC36-08GO28308; 679933; EP/S003053/1
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; lithium ion batteries; x-ray diffraction; computed tomography; crystallography
Citation Formats
Finegan, Donal P., Vamvakeros, Antonis, Tan, Chun, Heenan, Thomas M. M., Daemi, Sohrab R., Seitzman, Natalie, Di Michiel, Marco, Jacques, Simon, Beale, Andrew M., Brett, Dan J. L., Shearing, Paul R., and Smith, Kandler. Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes. United States: N. p., 2020.
Web. doi:10.1038/s41467-020-14467-x.
Finegan, Donal P., Vamvakeros, Antonis, Tan, Chun, Heenan, Thomas M. M., Daemi, Sohrab R., Seitzman, Natalie, Di Michiel, Marco, Jacques, Simon, Beale, Andrew M., Brett, Dan J. L., Shearing, Paul R., & Smith, Kandler. Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes. United States. https://doi.org/10.1038/s41467-020-14467-x
Finegan, Donal P., Vamvakeros, Antonis, Tan, Chun, Heenan, Thomas M. M., Daemi, Sohrab R., Seitzman, Natalie, Di Michiel, Marco, Jacques, Simon, Beale, Andrew M., Brett, Dan J. L., Shearing, Paul R., and Smith, Kandler. Fri .
"Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes". United States. https://doi.org/10.1038/s41467-020-14467-x. https://www.osti.gov/servlets/purl/1601577.
@article{osti_1601577,
title = {Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes},
author = {Finegan, Donal P. and Vamvakeros, Antonis and Tan, Chun and Heenan, Thomas M. M. and Daemi, Sohrab R. and Seitzman, Natalie and Di Michiel, Marco and Jacques, Simon and Beale, Andrew M. and Brett, Dan J. L. and Shearing, Paul R. and Smith, Kandler},
abstractNote = {The performance of lithium ion electrodes is hindered by unfavorable chemical heterogeneities that pre-exist or develop during operation. Time-resolved spatial descriptions are needed to understand the link between such heterogeneities and a cell's performance. Here, operando high-resolution X-ray diffraction-computed tomography is used to spatially and temporally quantify crystallographic heterogeneities within and between particles throughout both fresh and degraded LixMn2O4 electrodes. This imaging technique facilitates identification of stoichiometric differences between particles and stoichiometric gradients and phase heterogeneities within particles. Through radial quantification of phase fractions, the response of distinct particles to lithiation is found to vary; most particles contain localized regions that transition to rock salt LiMnO2 within the first cycle. Other particles contain monoclinic Li2MnO3 near the surface and almost pure spinel LixMn2O4 near the core. Following 150 cycles, concentrations of LiMnO2 and Li2MnO3 significantly increase and widely vary between particles.},
doi = {10.1038/s41467-020-14467-x},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Fri Jan 31 00:00:00 EST 2020},
month = {Fri Jan 31 00:00:00 EST 2020}
}
Web of Science
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