Fundamental Insights from a Single-Crystal Sodium Iridate Battery
Abstract
Electrochemically driven chemical transformations play the key role in controlling storage of energy in chemical bonds and subsequent conversion to power electric vehicles and consumer electronics. The promise of coupling anionic oxygen redox with cationic redox to achieve a substantial increase in capacities has inspired research in a wide range of electrode materials. A key challenge is that these studies have focused on polycrystalline materials, where it is hard to perform precise structural determinations, especially related to the location of light atoms. Here a different approach is utilized and a highly ordered single crystal, Na2-xIrO3 is harnessed, to explore the role of defects and structural transformations in layered transition metal oxide materials on redox-activity, capacity, reversibility, and stability. Within a combined experimental and theoretical framework, it is demonstrated that 1) it is possible to cycle Na2-xIrO3, offering proof of principle for single-crystal based batteries 2) structural phase transitions coincide with Ir4+/Ir5+ redox couple with no evident contribution from anionic redox 3) strong irreversibility and capacity fade observed during cycling correlates with the Na+ migration resulting in progressive growth of an electrochemically inert O3-type NaIrO3 phase.
- Authors:
-
[1];
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
- Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Univ. of Illinois, Chicago, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1631973
- Alternate Identifier(s):
- OSTI ID: 1598057
- Grant/Contract Number:
- AC02-06CH11357; AC02‐06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 10; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; electrochemical synthesis; oxygen redox; polycrystalline powders; single-crystals; structural and redox behavior; structural defects
Citation Formats
Tepavcevic, Sanja, Zheng, Hong, Hinks, David G., Key, Baris, Ward, Logan, Lu, Zhi, Stoumpos, Costas, Ren, Yang, Freeland, John W., Wolverton, Christopher, Phillips, Patrick, Klie, Robert, Mitchell, John F., and Markovic, Nenad M. Fundamental Insights from a Single-Crystal Sodium Iridate Battery. United States: N. p., 2020.
Web. doi:10.1002/aenm.201903128.
Tepavcevic, Sanja, Zheng, Hong, Hinks, David G., Key, Baris, Ward, Logan, Lu, Zhi, Stoumpos, Costas, Ren, Yang, Freeland, John W., Wolverton, Christopher, Phillips, Patrick, Klie, Robert, Mitchell, John F., & Markovic, Nenad M. Fundamental Insights from a Single-Crystal Sodium Iridate Battery. United States. https://doi.org/10.1002/aenm.201903128
Tepavcevic, Sanja, Zheng, Hong, Hinks, David G., Key, Baris, Ward, Logan, Lu, Zhi, Stoumpos, Costas, Ren, Yang, Freeland, John W., Wolverton, Christopher, Phillips, Patrick, Klie, Robert, Mitchell, John F., and Markovic, Nenad M. Tue .
"Fundamental Insights from a Single-Crystal Sodium Iridate Battery". United States. https://doi.org/10.1002/aenm.201903128. https://www.osti.gov/servlets/purl/1631973.
@article{osti_1631973,
title = {Fundamental Insights from a Single-Crystal Sodium Iridate Battery},
author = {Tepavcevic, Sanja and Zheng, Hong and Hinks, David G. and Key, Baris and Ward, Logan and Lu, Zhi and Stoumpos, Costas and Ren, Yang and Freeland, John W. and Wolverton, Christopher and Phillips, Patrick and Klie, Robert and Mitchell, John F. and Markovic, Nenad M.},
abstractNote = {Electrochemically driven chemical transformations play the key role in controlling storage of energy in chemical bonds and subsequent conversion to power electric vehicles and consumer electronics. The promise of coupling anionic oxygen redox with cationic redox to achieve a substantial increase in capacities has inspired research in a wide range of electrode materials. A key challenge is that these studies have focused on polycrystalline materials, where it is hard to perform precise structural determinations, especially related to the location of light atoms. Here a different approach is utilized and a highly ordered single crystal, Na2-xIrO3 is harnessed, to explore the role of defects and structural transformations in layered transition metal oxide materials on redox-activity, capacity, reversibility, and stability. Within a combined experimental and theoretical framework, it is demonstrated that 1) it is possible to cycle Na2-xIrO3, offering proof of principle for single-crystal based batteries 2) structural phase transitions coincide with Ir4+/Ir5+ redox couple with no evident contribution from anionic redox 3) strong irreversibility and capacity fade observed during cycling correlates with the Na+ migration resulting in progressive growth of an electrochemically inert O3-type NaIrO3 phase.},
doi = {10.1002/aenm.201903128},
journal = {Advanced Energy Materials},
number = 10,
volume = 10,
place = {United States},
year = {Tue Mar 10 00:00:00 EDT 2020},
month = {Tue Mar 10 00:00:00 EDT 2020}
}
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