Mutual modulation between surface chemistry and bulk microstructure within secondary particles of nickel-rich layered oxides

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dc.contributor.authorLi, Shaofengen
dc.contributor.authorJiang, Zhisenen
dc.contributor.authorHan, Jiaxiuen
dc.contributor.authorXu, Zhengruien
dc.contributor.authorWang, Chenxuen
dc.contributor.authorHuang, Haien
dc.contributor.authorYu, Changen
dc.contributor.authorLee, Sang-Junen
dc.contributor.authorPianetta, Pieroen
dc.contributor.authorOhldag, Hendriken
dc.contributor.authorQiu, Jieshanen
dc.contributor.authorLee, Jun-Siken
dc.contributor.authorLin, Fengen
dc.contributor.authorZhao, Kejieen
dc.contributor.authorLiu, Yijinen
dc.contributor.departmentChemistryen
dc.date.accessioned2021-02-08T20:02:36Zen
dc.date.available2021-02-08T20:02:36Zen
dc.date.issued2020-09-07en
dc.description.abstractSurface lattice reconstruction is commonly observed in nickel-rich layered oxide battery cathode materials, causing unsatisfactory high-voltage cycling performance. However, the interplay of the surface chemistry and the bulk microstructure remains largely unexplored due to the intrinsic structural complexity and the lack of integrated diagnostic tools for a thorough investigation at complementary length scales. Herein, by combining nano-resolution X-ray probes in both soft and hard X-ray regimes, we demonstrate correlative surface chemical mapping and bulk microstructure imaging over a single charged LiNi0.8Mn0.1Co0.1O2 (NMC811) secondary particle. We reveal that the sub-particle regions with more micro cracks are associated with more severe surface degradation. A mechanism of mutual modulation between the surface chemistry and the bulk microstructure is formulated based on our experimental observations and finite element modeling. Such a surface-to-bulk reaction coupling effect is fundamentally important for the design of the next generation battery cathode materials.en
dc.description.notesUse of SSRL, SLAC National Accelerator Laboratory, is supported by the U.S. DOE, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. F.L. acknowledges support from the National Science Foundation under Grant No. DMR-1832613. J.H. and K.Z. are grateful for the support by the National Science Foundation through the grants CMMI-1726392 and DMR-1832707. The NMC electrodes were produced at the U.S. DOE's 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. S.L. acknowledges the support from the Chinese Scholarship Council (No. 201806060018). The engineering support from D. Van Campen, D. Day and V. Borzenets for the TXM experiment at beamline 6-2c of SSRL is gratefully acknowledged.en
dc.description.sponsorshipU.S. DOE, Office of Science, Office of Basic Energy SciencesUnited States Department of Energy (DOE) [DE-AC02-76SF00515]; National Science FoundationNational Science Foundation (NSF) [CMMI-1726392, DMR-1832707, DMR-1832613]; DOE Vehicle Technologies Program (VTP) within the core funding of the Applied Battery Research (ABR) for Transportation ProgramUnited States Department of Energy (DOE); Chinese Scholarship CouncilChina Scholarship Council [201806060018]en
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1038/s41467-020-18278-yen
dc.identifier.issn2041-1723en
dc.identifier.issue1en
dc.identifier.other4433en
dc.identifier.pmid32895388en
dc.identifier.urihttp://hdl.handle.net/10919/102312en
dc.identifier.volume11en
dc.language.isoenen
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.titleMutual modulation between surface chemistry and bulk microstructure within secondary particles of nickel-rich layered oxidesen
dc.title.serialNature Communicationsen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.dcmitypeStillImageen

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