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Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts
Abstract
Cation-disordered rock salts (DRXs) are well known for their potential to realize the goal of achieving scalable Ni- and Co-free high-energy-density Li-ion batteries. Unlike in most cathode materials, the disordered cation distribution may lead to more factors that control the electrochemistry of DRXs. An important variable that is not emphasized by research community is regarding whether a DRX exists in a more thermodynamically stable form or a more metastable form. Moreover, within the scope of metastable DRXs, over-stoichiometric DRXs, which allow relaxation of the site balance constraint of a rock salt structure, are particularly underexplored. In this work, these findings are reported in locating a generally applicable approach to “metastabilize” thermodynamically stable Mn-based DRXs to metastable ones by introducing Li over-stoichiometry. Further, the over-stoichiometric metastabilization greatly stimulates more redox activities, enables better reversibility of Li deintercalation/intercalation, and changes the energy storage mechanism. The metastabilized DRXs can be transformed back to the thermodynamically stable form, which also reverts the electrochemical properties, further contrasting the two categories of DRXs. This work enriches the structural and compositional space of DRX families and adds new pathways for rationally tuning the properties of DRX cathodes.
- Authors:
-
[1]
- Univ. of New Mexico, Albuquerque, NM (United States)
- Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights, NSW (Australia); Univ. of Sydney, NSW (Australia)
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- South Dakota School of Mines and Technology, Rapid City, SD (United States)
- Albuquerque Institute for Math & Science, Albuquerque, NM (United States)
- Spallation Neutron Source Science Center, Dongguan (China); Chinese Academy of Sciences (CAS), Beijing (China). Inst. of High Energy Physics (IHEP)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF)
- OSTI Identifier:
- 2308898
- Grant/Contract Number:
- AC02-76SF00515; 2154617
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 35; Journal Issue: 51; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; cation-disordered rock salts; Li-ion batteries; metastability; over-stoichiometry
Citation Formats
Wang, You, Outka, Alexandra, Takele, Wassie Mersha, Avdeev, Maxim, Sainio, Sami, Liu, Rui, Kee, Vanessa, Choe, Wonu, Raji‐Adefila, Basirat, Nordlund, Dennis, Zhou, Shan, Kan, Wang Hay, Habteyes, Terefe G., and Chen, Dongchang. Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts. United States: N. p., 2023.
Web. doi:10.1002/adma.202306396.
Wang, You, Outka, Alexandra, Takele, Wassie Mersha, Avdeev, Maxim, Sainio, Sami, Liu, Rui, Kee, Vanessa, Choe, Wonu, Raji‐Adefila, Basirat, Nordlund, Dennis, Zhou, Shan, Kan, Wang Hay, Habteyes, Terefe G., & Chen, Dongchang. Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts. United States. https://doi.org/10.1002/adma.202306396
Wang, You, Outka, Alexandra, Takele, Wassie Mersha, Avdeev, Maxim, Sainio, Sami, Liu, Rui, Kee, Vanessa, Choe, Wonu, Raji‐Adefila, Basirat, Nordlund, Dennis, Zhou, Shan, Kan, Wang Hay, Habteyes, Terefe G., and Chen, Dongchang. Tue .
"Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts". United States. https://doi.org/10.1002/adma.202306396.
@article{osti_2308898,
title = {Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts},
author = {Wang, You and Outka, Alexandra and Takele, Wassie Mersha and Avdeev, Maxim and Sainio, Sami and Liu, Rui and Kee, Vanessa and Choe, Wonu and Raji‐Adefila, Basirat and Nordlund, Dennis and Zhou, Shan and Kan, Wang Hay and Habteyes, Terefe G. and Chen, Dongchang},
abstractNote = {Cation-disordered rock salts (DRXs) are well known for their potential to realize the goal of achieving scalable Ni- and Co-free high-energy-density Li-ion batteries. Unlike in most cathode materials, the disordered cation distribution may lead to more factors that control the electrochemistry of DRXs. An important variable that is not emphasized by research community is regarding whether a DRX exists in a more thermodynamically stable form or a more metastable form. Moreover, within the scope of metastable DRXs, over-stoichiometric DRXs, which allow relaxation of the site balance constraint of a rock salt structure, are particularly underexplored. In this work, these findings are reported in locating a generally applicable approach to “metastabilize” thermodynamically stable Mn-based DRXs to metastable ones by introducing Li over-stoichiometry. Further, the over-stoichiometric metastabilization greatly stimulates more redox activities, enables better reversibility of Li deintercalation/intercalation, and changes the energy storage mechanism. The metastabilized DRXs can be transformed back to the thermodynamically stable form, which also reverts the electrochemical properties, further contrasting the two categories of DRXs. This work enriches the structural and compositional space of DRX families and adds new pathways for rationally tuning the properties of DRX cathodes.},
doi = {10.1002/adma.202306396},
journal = {Advanced Materials},
number = 51,
volume = 35,
place = {United States},
year = {Tue Oct 31 00:00:00 EDT 2023},
month = {Tue Oct 31 00:00:00 EDT 2023}
}
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