Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts

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

doi:10.1002/adma.202306396

Title: Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts

Journal Article · 30 October 2023 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202306396 · OSTI ID:2308898

Wang, You ^[1]; Outka, Alexandra ^[2]; Takele, Wassie Mersha ^[2]; Avdeev, Maxim ^[3]; Sainio, Sami ^[4]; Liu, Rui ^[2]; Kee, Vanessa ^[5]; Choe, Wonu ^[6]; Raji‐Adefila, Basirat ^[2]; Nordlund, Dennis ^[4]; Zhou, Shan ^[5]; Kan, Wang Hay ^[7]; Habteyes, Terefe G. ^[2];

^[2]

Univ. of New Mexico, Albuquerque, NM (United States); SLAC
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)

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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2308898

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 51 Vol. 35; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
Li-ion batteries
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metastability
over-stoichiometry

Title: Over-Stoichiometric Metastabilization of Cation-Disordered Rock Salts

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