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      Eliminating interfacial O-involving degradation in Li-rich Mn-based cathodes for all-solid-state lithium batteries

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          Abstract

          In the pursuit of energy-dense all-solid-state lithium batteries (ASSBs), Li-rich Mn-based oxide (LRMO) cathodes provide an exciting path forward with unexpectedly high capacity, low cost, and excellent processibility. However, the cause for LRMO|solid electrolyte interfacial degradation remains a mystery, hindering the application of LRMO-based ASSBs. Here, we first reveal that the surface oxygen instability of LRMO is the driving force for interfacial degradation, which severely blocks the interfacial Li-ion transport and triggers fast battery failure. By replacing the charge compensation of surface oxygen with sulfite, the overoxidation and interfacial degradation can be effectively prevented, therefore achieving a high specific capacity (~248 mAh g −1, 1.1 mAh cm −2; ~225 mAh g −1, 2.9 mAh cm −2) and excellent long-term cycling stability of >300 cycles with 81.2% capacity retention at room temperature. These findings emphasize the importance of irreversible anion reactions in interfacial failure and provide fresh insights into constructing stable interfaces in LRMO-based ASSBs.

          Abstract

          Abstract

          Li-rich Mn-based cathode interfaces were designed to inhibit the O-involving degradation for energy-dense lithium batteries.

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          Most cited references50

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                Author and article information

                Contributors
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SoftwareRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Role: Investigation
                Role: Formal analysisRole: MethodologyRole: ResourcesRole: SoftwareRole: Visualization
                Role: Formal analysisRole: InvestigationRole: Resources
                Role: InvestigationRole: ResourcesRole: Validation
                Role: Formal analysisRole: InvestigationRole: Resources
                Role: Formal analysis
                Role: ConceptualizationRole: Funding acquisitionRole: SupervisionRole: Writing - review & editing
                Role: ConceptualizationRole: Funding acquisitionRole: Project administrationRole: ResourcesRole: Supervision
                Role: ConceptualizationRole: Data curationRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: SoftwareRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Journal
                Sci Adv
                Sci Adv
                sciadv
                advances
                Science Advances
                American Association for the Advancement of Science
                2375-2548
                November 2022
                25 November 2022
                : 8
                : 47
                : eadd5189
                Affiliations
                [ 1 ]Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
                [ 2 ]State Key Laboratory of Automotive Safety and Energy, School of Vehicle and Mobility, Tsinghua University, Beijing 100084, China.
                [ 3 ]Advanced Research Institute for Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China.
                [ 4 ]Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.
                Author notes
                [* ]Corresponding author. Email: zcz@ 123456mail.tsinghua.edu.cn (C.-Z.Z.); zhang-qiang@ 123456mails.tsinghua.edu.cn (Q.Z.)
                Author information
                https://orcid.org/0000-0001-7724-3906
                https://orcid.org/0000-0002-1794-3086
                https://orcid.org/0000-0001-7565-2204
                https://orcid.org/0000-0001-8779-9086
                https://orcid.org/0000-0002-7686-6308
                https://orcid.org/0000-0002-0946-7155
                https://orcid.org/0000-0001-9442-3407
                https://orcid.org/0000-0001-8860-093X
                https://orcid.org/0000-0001-7394-9186
                https://orcid.org/0000-0002-3929-1541
                Article
                add5189
                10.1126/sciadv.add5189
                9699669
                36427308
                fc06525a-753f-4e5e-8279-d02bd38eb45b
                Copyright © 2022 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).

                This is an open-access article distributed under the terms of the Creative Commons Attribution license, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

                History
                : 16 June 2022
                : 06 October 2022
                Funding
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: 22108151
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: 22075029
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: 21805161
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: 21808124
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: 21825501
                Funded by: FundRef http://dx.doi.org/10.13039/501100004826, Natural Science Foundation of Beijing Municipality;
                Award ID: U1801257
                Funded by: FundRef http://dx.doi.org/10.13039/501100004826, Natural Science Foundation of Beijing Municipality;
                Award ID: BX2021135
                Funded by: FundRef http://dx.doi.org/10.13039/501100004826, Natural Science Foundation of Beijing Municipality;
                Award ID: 2021TQ0164
                Funded by: FundRef http://dx.doi.org/10.13039/501100004826, Natural Science Foundation of Beijing Municipality;
                Award ID: 2021M701827
                Funded by: FundRef http://dx.doi.org/10.13039/501100004826, Natural Science Foundation of Beijing Municipality;
                Award ID: Z20J00043
                Funded by: FundRef http://dx.doi.org/10.13039/501100013290, National Key Research and Development Program of China Stem Cell and Translational Research;
                Award ID: 2021YFB2500300
                Categories
                Research Article
                Physical and Materials Sciences
                SciAdv r-articles
                Chemistry
                Materials Science
                Chemistry
                Custom metadata
                Anne Suarez

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