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Tailoring Disordered/Ordered Phases to Revisit the Degradation Mechanism of High-Voltage LiNi0.5Mn1.5O4 Spinel Cathode Materials

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dc.contributor.authorSun, Huabinen
dc.contributor.authorHu, Anyangen
dc.contributor.authorSpence, Stephanieen
dc.contributor.authorKuai, Chunguangen
dc.contributor.authorHou, Dongen
dc.contributor.authorMu, Linqinen
dc.contributor.authorLiu, Jueen
dc.contributor.authorLi, Luxien
dc.contributor.authorSun, Chengjunen
dc.contributor.authorSainio, Samien
dc.contributor.authorNordlund, Dennisen
dc.contributor.authorLuo, Weien
dc.contributor.authorHuang, Yunhuien
dc.contributor.authorLin, Fengen
dc.date.accessioned2022-07-22T16:58:41Zen
dc.date.available2022-07-22T16:58:41Zen
dc.date.issued2022-05en
dc.description.abstractIn the spinel oxide cathode family, LiNi0.5Mn1.5O4 (LNMO) shows a high operating voltage (approximate to 4.7 V vs Li/Li+) and excellent Li-ion mobility with stable 3D conducting channels. Ni/Mn cation disordered and ordered phases usually coexist in LNMO materials, and they have distinct structural and electrochemical properties, resulting in different battery performances for LNMO materials with different phase compositions. Identifying the correlation between phase compositions and electrochemical properties is of significance to the improvement of battery performance and understanding of degradation mechanisms. Herein, the disordered/ordered phase compositions in LNMO materials are tailored by post-annealing strategies and their impacts on electrochemical performance and degradation mechanisms from the surface to the bulk are systematically investigated. The ordered phase increases rapidly as Mn3+ is oxidized to Mn4+ through a post-annealing process. LNMO with an intermediate fraction of disordered and ordered phases gives rise to improved cycling stability. This article further reports that a high ordered phase fraction can preferentially protect Ni from dissolution during cycling. However, these results suggest that the transition metal dissolution and surface structural change of LNMO do not exhibit a direct correlation with cycling stability. These results indicate the capacity fading mainly correlates with the bulk structural distortion, leading to decreased Li-ion kinetics.en
dc.description.notesThe work at Virginia Tech was supported by Department of Chemistry startup funds. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The pristine LNMO powder was produced at the U.S. Department of Energy's (DOE) CAMP (Cell Analysis, Modeling and Prototyping) Facility, Argonne National Laboratory. The CAMP Facility is fully supported by the DOE Vehicle Technologies Program (VTP) within the core funding of the Applied Battery Research (ABR) for Transportation Program. This research used resources of the Advanced Photon Sources at Argonne National Laboratory, which is a U.S. DOE Office of Science User Facility under contract No. DE-AC02-06CH11357. The use of the Spallation Neutron Source at Oak Ridge National Laboratory was supported by the U.S. DOE Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC05-00OR22725. This research used resources of the Advanced Light Source at Lawrence Berkeley National Laboratory, which is a U.S. DOE Office of Science User Facility under contract No. DE-AC02-05CH11231. The authors thank Dr. Gi-Hyeok Lee and Dr. Wanli Yang for fruitful discussion and soft XAS experiments. S.S. acknowledges funding from the Walter Ahlstrom Foundation. S.S. received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skodowska-Curie grant agreement No 841621.en
dc.description.sponsorshipDepartment of Chemistry startup funds; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]; Applied Battery Research (ABR) for Transportation Program; U.S. DOE Office of Science, Office of Basic Energy Sciences [DE-AC05-00OR22725]; U.S. DOE Office of Science User Facility [DE-AC02-05CH11231]; Walter Ahlstrom Foundation; European Union's Horizon 2020 research and innovation programme under the Marie Skodowska-Curie grant [841621]en
dc.description.versionPublished versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1002/adfm.202112279en
dc.identifier.eissn1616-3028en
dc.identifier.issn1616-301Xen
dc.identifier.issue21en
dc.identifier.other2112279en
dc.identifier.urihttp://hdl.handle.net/10919/111320en
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.subjectcycle lifeen
dc.subjectdisorder-to-order transitionen
dc.subjectfading mechanismen
dc.subjectmetal dissolutionen
dc.subjectspinel cathodesen
dc.titleTailoring Disordered/Ordered Phases to Revisit the Degradation Mechanism of High-Voltage LiNi0.5Mn1.5O4 Spinel Cathode Materialsen
dc.title.serialAdvanced Functional Materialsen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten

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