A reversible phase transition for sodium insertion in anatase TiO2
Abstract
Anatase TiO2 is a potential negative electrode for sodium-ion batteries. The sodium storage mechanism is, however, still under debate, yet its comprehension is required to optimize the electrochemical properties. To clarify the sodium storage mechanism occurring in anatase, we have used both electrochemical and chemical routes from which we obtained similar trends. During the first discharge, an irreversible plateau region is observed which corresponds to the insertion of Na+ within the interstitial sites of anatase and is accompanied by a drastic loss of the long-range order as revealed by X-ray diffraction, high resolution of high angle annular dark-field scanning transmission electron microscope (HAADF-STEM), and pair distribution function (PDF) analysis. Further structural analysis of the total scattering data indicates that the sodiated phase displays a layered-like rhombohedral R3m structure built from the stacking of Ti and Na slabs. Because of the initial 3D network of anatase, the reduced phase shows strong disorder due to cationic intermixing between the Ti and Na slabs and the refined chemical formula is (Na0.43Ti0.57)3a 0.22Na0.39Ti0.39)3bO2, where refers to vacancy. The presence of high valence Ti ions in the Na layers induces a contraction of the c-parameter as compared to the ordered phase. Upon desodiation, the structuremore »
- Authors:
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- European Commission - Community Research and Development Information Service (CORDIS) - Seventh Framework Programme (FP7); Engineering and Physical Sciences Research Council (EPSRC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division
- OSTI Identifier:
- 1372078
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 4; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; NaTiO2; disordered layered structure; pair distribution function; sodium-ion batteries
Citation Formats
Li, Wei, Fukunishi, Mika, Morgan, Benjamin J., Borkiewicz, Olaf J., Chapman, Karena W., Pralong, Valerie, Maignan, Antoine, Lebedev, Oleg I., Ma, Jiwei, Groult, Henri, Komaba, Shinichi, and Dambournet, Damien. A reversible phase transition for sodium insertion in anatase TiO2. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.7b00098.
Li, Wei, Fukunishi, Mika, Morgan, Benjamin J., Borkiewicz, Olaf J., Chapman, Karena W., Pralong, Valerie, Maignan, Antoine, Lebedev, Oleg I., Ma, Jiwei, Groult, Henri, Komaba, Shinichi, & Dambournet, Damien. A reversible phase transition for sodium insertion in anatase TiO2. United States. https://doi.org/10.1021/acs.chemmater.7b00098
Li, Wei, Fukunishi, Mika, Morgan, Benjamin J., Borkiewicz, Olaf J., Chapman, Karena W., Pralong, Valerie, Maignan, Antoine, Lebedev, Oleg I., Ma, Jiwei, Groult, Henri, Komaba, Shinichi, and Dambournet, Damien. Tue .
"A reversible phase transition for sodium insertion in anatase TiO2". United States. https://doi.org/10.1021/acs.chemmater.7b00098. https://www.osti.gov/servlets/purl/1372078.
@article{osti_1372078,
title = {A reversible phase transition for sodium insertion in anatase TiO2},
author = {Li, Wei and Fukunishi, Mika and Morgan, Benjamin J. and Borkiewicz, Olaf J. and Chapman, Karena W. and Pralong, Valerie and Maignan, Antoine and Lebedev, Oleg I. and Ma, Jiwei and Groult, Henri and Komaba, Shinichi and Dambournet, Damien},
abstractNote = {Anatase TiO2 is a potential negative electrode for sodium-ion batteries. The sodium storage mechanism is, however, still under debate, yet its comprehension is required to optimize the electrochemical properties. To clarify the sodium storage mechanism occurring in anatase, we have used both electrochemical and chemical routes from which we obtained similar trends. During the first discharge, an irreversible plateau region is observed which corresponds to the insertion of Na+ within the interstitial sites of anatase and is accompanied by a drastic loss of the long-range order as revealed by X-ray diffraction, high resolution of high angle annular dark-field scanning transmission electron microscope (HAADF-STEM), and pair distribution function (PDF) analysis. Further structural analysis of the total scattering data indicates that the sodiated phase displays a layered-like rhombohedral R3m structure built from the stacking of Ti and Na slabs. Because of the initial 3D network of anatase, the reduced phase shows strong disorder due to cationic intermixing between the Ti and Na slabs and the refined chemical formula is (Na0.43Ti0.57)3a 0.22Na0.39Ti0.39)3bO2, where refers to vacancy. The presence of high valence Ti ions in the Na layers induces a contraction of the c-parameter as compared to the ordered phase. Upon desodiation, the structure further amorphized and the local structure probed by PDF is shown to be similar to the anatase TiO2, suggesting that the 3D network is recovered. The reversible sodium insertion/deinsertion is thus attributed to the rhombohedral active phase formed during the first discharge, and an oxidized phase featuring the local structure of anatase. Due to the amorphous nature of the two phases, the potential-composition curves are characterized by a sloping curve. Lastly, a comparison between the intercalation of lithium and sodium into anatase TiO2 performed by DFT calculations confirmed that, for the sodiated phase, the rhombohedral structure is more stable than the tetragonal phase observed during the lithiation of nanoparticles.},
doi = {10.1021/acs.chemmater.7b00098},
journal = {Chemistry of Materials},
number = 4,
volume = 29,
place = {United States},
year = {Tue Feb 07 00:00:00 EST 2017},
month = {Tue Feb 07 00:00:00 EST 2017}
}
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Figures / Tables:
Figure 1: Galvanostatic discharge-charge curves of Na//TiO2 cells. The cells were cycled at 10 mA.g-1.
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