Multi-Stage Structural Transformations in Zero-Strain Lithium Titanate Unveiled by in Situ X-ray Absorption Fingerprints
Abstract
Zero-strain electrodes, such as spinel lithium titanate (Li4/3Ti5/3O4), are appealing for application in batteries due to their negligible volume change and extraordinary stability upon repeated charge/discharge cycles. On the other hand, this same property makes it challenging to probe their structural changes during the electrochemical reaction. Herein, we report in situ studies of lithiation-driven structural transformations in Li4/3Ti5/3O4 via a combination of X-ray absorption spectroscopy and ab initio calculations. Based on excellent agreement between computational and experimental spectra of Ti K-edge, we identified key spectral features as fingerprints for quantitative assessment of structural evolution at different length scales. Results from this study indicate that, despite the small variation in the crystal lattice during lithiation, pronounced structural transformations occur in Li4/3Ti5/3O4, both locally and globally, giving rise to a multi-stage kinetic process involving mixed quasi-solid solution/macroscopic two-phase transformations over a wide range of Li concentrations. This work highlights the unique capability of combining in situ core-level spectroscopy and first-principles calculations for probing Li-ion intercalation in zero-strain electrodes, which is crucial to designing high-performance electrode materials for long-life batteries.
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Stony Brook Univ., NY (United States). Dept. of Chemistry
- Brookhaven National Lab. (BNL), Upton, NY (United States). Energy and Photon Sciences Directorate
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
- Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
- Stony Brook Univ., NY (United States). Dept. of Chemistry. Dept. of Materials Science and Chemical Engineering
- Stony Brook Univ., NY (United States). Dept. of Chemistry. Dept. of Materials Science and Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Energy and Photon Sciences Directorate
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2M); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2mt); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); BNL Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1439804
- Alternate Identifier(s):
- OSTI ID: 1489025
- Report Number(s):
- BNL-114533-2017-JAAM
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- SC0012704; SC0012673; FG02-03ER15476; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 139; Journal Issue: 46; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhang, Wei, Topsakal, Mehmet, Cama, Christina, Pelliccione, Christopher J., Zhao, Hu, Ehrlich, Steven, Wu, Lijun, Zhu, Yimei, Frenkel, Anatoly I., Takeuchi, Kenneth J., Takeuchi, Esther S., Marschilok, Amy C., Lu, Deyu, and Wang, Feng. Multi-Stage Structural Transformations in Zero-Strain Lithium Titanate Unveiled by in Situ X-ray Absorption Fingerprints. United States: N. p., 2017.
Web. doi:10.1021/jacs.7b07628.
Zhang, Wei, Topsakal, Mehmet, Cama, Christina, Pelliccione, Christopher J., Zhao, Hu, Ehrlich, Steven, Wu, Lijun, Zhu, Yimei, Frenkel, Anatoly I., Takeuchi, Kenneth J., Takeuchi, Esther S., Marschilok, Amy C., Lu, Deyu, & Wang, Feng. Multi-Stage Structural Transformations in Zero-Strain Lithium Titanate Unveiled by in Situ X-ray Absorption Fingerprints. United States. https://doi.org/10.1021/jacs.7b07628
Zhang, Wei, Topsakal, Mehmet, Cama, Christina, Pelliccione, Christopher J., Zhao, Hu, Ehrlich, Steven, Wu, Lijun, Zhu, Yimei, Frenkel, Anatoly I., Takeuchi, Kenneth J., Takeuchi, Esther S., Marschilok, Amy C., Lu, Deyu, and Wang, Feng. Fri .
"Multi-Stage Structural Transformations in Zero-Strain Lithium Titanate Unveiled by in Situ X-ray Absorption Fingerprints". United States. https://doi.org/10.1021/jacs.7b07628. https://www.osti.gov/servlets/purl/1439804.
@article{osti_1439804,
title = {Multi-Stage Structural Transformations in Zero-Strain Lithium Titanate Unveiled by in Situ X-ray Absorption Fingerprints},
author = {Zhang, Wei and Topsakal, Mehmet and Cama, Christina and Pelliccione, Christopher J. and Zhao, Hu and Ehrlich, Steven and Wu, Lijun and Zhu, Yimei and Frenkel, Anatoly I. and Takeuchi, Kenneth J. and Takeuchi, Esther S. and Marschilok, Amy C. and Lu, Deyu and Wang, Feng},
abstractNote = {Zero-strain electrodes, such as spinel lithium titanate (Li4/3Ti5/3O4), are appealing for application in batteries due to their negligible volume change and extraordinary stability upon repeated charge/discharge cycles. On the other hand, this same property makes it challenging to probe their structural changes during the electrochemical reaction. Herein, we report in situ studies of lithiation-driven structural transformations in Li4/3Ti5/3O4 via a combination of X-ray absorption spectroscopy and ab initio calculations. Based on excellent agreement between computational and experimental spectra of Ti K-edge, we identified key spectral features as fingerprints for quantitative assessment of structural evolution at different length scales. Results from this study indicate that, despite the small variation in the crystal lattice during lithiation, pronounced structural transformations occur in Li4/3Ti5/3O4, both locally and globally, giving rise to a multi-stage kinetic process involving mixed quasi-solid solution/macroscopic two-phase transformations over a wide range of Li concentrations. This work highlights the unique capability of combining in situ core-level spectroscopy and first-principles calculations for probing Li-ion intercalation in zero-strain electrodes, which is crucial to designing high-performance electrode materials for long-life batteries.},
doi = {10.1021/jacs.7b07628},
journal = {Journal of the American Chemical Society},
number = 46,
volume = 139,
place = {United States},
year = {2017},
month = {10}
}
Web of Science
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