Over‐stoichiometric metastabilization of cation‐disordered rock salts

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dc.contributor.authorWang, Yen_AU
dc.contributor.authorOutka, Aen_AU
dc.contributor.authorTakele, WMen_AU
dc.contributor.authorAvdeev, Men_AU
dc.contributor.authorSainio, Sen_AU
dc.contributor.authorLiu, Ren_AU
dc.contributor.authorKee, Ven_AU
dc.contributor.authorChoe, Wen_AU
dc.contributor.authorRaji‐Adefila, Ben_AU
dc.contributor.authorNordlund, Den_AU
dc.contributor.authorZhou, Sen_AU
dc.contributor.authorKan, WHen_AU
dc.contributor.authorHabteyes, TGen_AU
dc.contributor.authorChen, DCen_AU
dc.date.accessioned2025-01-16T00:55:47Zen_AU
dc.date.available2025-01-16T00:55:47Zen_AU
dc.date.issued2023-12-21en_AU
dc.date.statistics2024-06-27en_AU
dc.descriptionThis work was financially supported by University of New Mexico new faculty startup award, research allocation committee award, and Oak Ridge Associated Universities Ralph E. Powe Junior Faculty Enhancement Award. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory is supported by the Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-76SF00515. Acquisition of the quantum cascade laser used for s-SNOM IR imaging in this work was supported by NSF award 2154617. S.Z. was supported by faculty startup award at South Dakota School of Mines and Technology. The ICP-MS instrument was supported in part by NIH P20GM130422 and P30ES032755. The authors greatly appreciate the neutron beamtime granted from ECHIDNA in ANSTO.en_AU
dc.description.abstractCation‐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. 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. © 1999-2024 John Wiley & Sons, Inc or related companies.en_AU
dc.format.mediumPrint-Electronicen_AU
dc.identifier.articlenumbere2306396en_AU
dc.identifier.citationWang, Y., Outka, A., Takele, W. M., Avdeev, M., Sainio, S., Liu, R., Kee, V., Choe, W., Raji-Adefila, B., Nordlund, D., Zhou, S., Kan, W. H., Habteyes, T. G., & Chen, D. (2023). Over-stoichiometric metastabilization of cation-disordered rock salts. Advanced Materials, 35(51), 2306396. doi:10.1002/adma.202306396en_AU
dc.identifier.issn0935-9648en_AU
dc.identifier.issn1521-4095en_AU
dc.identifier.issue51en_AU
dc.identifier.journaltitleAdvanced Materialsen_AU
dc.identifier.urihttps://doi.org/10.1002/adma.202306396en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15947en_AU
dc.identifier.volume35en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherWileyen_AU
dc.subjectSaltsen_AU
dc.subjectMetastable statesen_AU
dc.subjectNickelen_AU
dc.subjectLithium ion batteriesen_AU
dc.subjectCathodesen_AU
dc.subjectThermodynamicsen_AU
dc.subjectStoichiometryen_AU
dc.subjectEnergy storageen_AU
dc.subjectElectrochemistryen_AU
dc.titleOver‐stoichiometric metastabilization of cation‐disordered rock saltsen_AU
dc.typeJournal Articleen_AU
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