Investigating Particle Size-Dependent Redox Kinetics and Charge Distribution in Disordered Rocksalt Cathodes

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dc.contributor.authorZhang, Yuxinen
dc.contributor.authorHu, Anyangen
dc.contributor.authorLiu, Jueen
dc.contributor.authorXu, Zhengruien
dc.contributor.authorMu, Linqinen
dc.contributor.authorSainio, Samien
dc.contributor.authorNordlund, Dennisen
dc.contributor.authorLi, Luxien
dc.contributor.authorSun, Cheng-Junen
dc.contributor.authorXiao, Xianghuien
dc.contributor.authorLiu, Yijinen
dc.contributor.authorLin, Fengen
dc.date.accessioned2022-08-02T13:08:38Zen
dc.date.available2022-08-02T13:08:38Zen
dc.date.issued2022-04en
dc.description.abstractUnderstanding how various redox activities evolve and distribute in disordered rocksalt oxides (DRX) can advance insights into manipulating materials properties for achieving stable, high-energy batteries. Herein, the authors present how the reaction kinetics and spatial distribution of redox activities are governed by the particle size of DRX materials. The size-dependent electrochemical performance is attributed to the distinct cationic and anionic reaction kinetics at different sizes, which can be tailored to achieve optimal capacity and stability. Overall, the local charged domains in DRX particles display random heterogeneity caused by the isotropic delithiation pathways. Owing to the kinetic limitation, the micron-sized particles exhibit a holistic "core-shell" charge distribution, whereas sub-micron particles show more uniform redox reactions throughout the particles and ensembles. Sub-micron DRX particles exhibit increasing anionic redox activities yet inferior cycling stability. In summary, engineering particle size can effectively modulate how cationic and anionic redox activities evolve and distribute in DRX materials.en
dc.description.notesThe work was supported by the Thomas F. and Kate Miller Jeffress Memorial Trust, Bank of America, Trustee and the Jeffress Trust Awards Program in Interdisciplinary Research, and the National Science Foundation (DMR-2045570). Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. This research the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Research conducted at Spallation Neutron Source in Oak Ridge National Laboratory (NOMAD) was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. S.S. has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No. 841621. S.S. acknowledges funding from the Walter Ahlstrom Foundation. Y.Z. and F. L. thank Dr. X. Wang for the fruitful discussion.en
dc.description.sponsorshipThomas F. and Kate Miller Jeffress Memorial Trust; Bank of America; Jeffress Trust Awards Program in Interdisciplinary Research; National Science Foundation [DMR-2045570]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]; DOE Office of Science [DE-AC02-06CH11357, DE-SC0012704]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant [841621]; Walter Ahlstrom Foundationen
dc.description.versionPublished versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1002/adfm.202110502en
dc.identifier.eissn1616-3028en
dc.identifier.issn1616-301Xen
dc.identifier.issue17en
dc.identifier.other2110502en
dc.identifier.urihttp://hdl.handle.net/10919/111420en
dc.identifier.volume32en
dc.language.isoenen
dc.publisherWiley-V C H Verlagen
dc.rightsCreative Commons Attribution-NonCommercial 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by-nc/4.0/en
dc.subjectdisordered rocksalt cathodesen
dc.subjectheterogeneous charge distributionen
dc.subjectparticle size engineeringen
dc.subjectsize-dependent redox reactionsen
dc.titleInvestigating Particle Size-Dependent Redox Kinetics and Charge Distribution in Disordered Rocksalt Cathodesen
dc.title.serialAdvanced Functional Materialsen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten

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