Surface coating by mechanofusion modulates bulk charging pathways and battery performance of Ni-rich layered cathodes
Ni-rich layered oxides as high-capacity battery cathodes suffer from degradation at high voltages. We utilize a dry surface modification method, mechanofusion (MF), to achieve enhanced battery stability. The simplicity, high yield, and flexibility make it cost-effective and highly attractive for pro...
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| Veröffentlicht in: | Proceedings of the National Academy of Sciences - PNAS 2022-12, Vol.119 (49), p.e2212802119-e2212802119 |
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| creator | Hou, Dong Han, Jiaxiu Geng, Chenxi Xu, Zhengrui AlMarzooqi, Modhi M Zhang, Jin Yang, Zhijie Min, Jungki Xiao, Xianghui Borkiewicz, Olaf Wiaderek, Kamila Liu, Yijin Zhao, Kejie Lin, Feng |
| description | Ni-rich layered oxides as high-capacity battery cathodes suffer from degradation at high voltages. We utilize a dry surface modification method, mechanofusion (MF), to achieve enhanced battery stability. The simplicity, high yield, and flexibility make it cost-effective and highly attractive for processing at the industrial scale. The underlying mechanisms responsible for performance improvement are unveiled by a systematic study combining multiple probes, e.g., 3D nano-tomography, spectroscopic imaging, in situ synchrotron diffraction, and finite element analysis (FEA). MF affects the bulk crystallography by introducing partially disordered structure, microstrain, and local lattice variation. Furthermore, the crack initiation and propagation pattern during delithiation are regulated and the overall mechanical fracture is reduced after such surface coating. We validate that MF can alter the bulk charging pathways. Such a synergic effect between surface modification and bulk charge distribution is fundamentally important for designing next-generation battery cathode materials. |
| doi_str_mv | 10.1073/pnas.2212802119 |
| format | Article |
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We utilize a dry surface modification method, mechanofusion (MF), to achieve enhanced battery stability. The simplicity, high yield, and flexibility make it cost-effective and highly attractive for processing at the industrial scale. The underlying mechanisms responsible for performance improvement are unveiled by a systematic study combining multiple probes, e.g., 3D nano-tomography, spectroscopic imaging, in situ synchrotron diffraction, and finite element analysis (FEA). MF affects the bulk crystallography by introducing partially disordered structure, microstrain, and local lattice variation. Furthermore, the crack initiation and propagation pattern during delithiation are regulated and the overall mechanical fracture is reduced after such surface coating. We validate that MF can alter the bulk charging pathways. Such a synergic effect between surface modification and bulk charge distribution is fundamentally important for designing next-generation battery cathode materials.</description><identifier>ISSN: 0027-8424</identifier><identifier>EISSN: 1091-6490</identifier><identifier>DOI: 10.1073/pnas.2212802119</identifier><identifier>PMID: 36454748</identifier><language>eng</language><publisher>United States: National Academy of Sciences</publisher><subject>Batteries ; Cathodes ; Charge distribution ; charge heterogeneity ; Charging ; coating ; Crack initiation ; Crack propagation ; Crystallography ; Electrode materials ; ENERGY STORAGE ; Finite element method ; in situ XRD ; Microstrain ; Physical Sciences ; rechargeable batteries ; Synchrotrons ; tomography</subject><ispartof>Proceedings of the National Academy of Sciences - PNAS, 2022-12, Vol.119 (49), p.e2212802119-e2212802119</ispartof><rights>Copyright National Academy of Sciences Dec 6, 2022</rights><rights>Copyright © 2022 the Author(s). Published by PNAS. 2022</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c514t-8672015dddac62093ec00925890504fea6aa908f923275473e68458638dd718a3</citedby><cites>FETCH-LOGICAL-c514t-8672015dddac62093ec00925890504fea6aa908f923275473e68458638dd718a3</cites><orcidid>0000-0002-3729-3148 ; 0000-0002-8417-2488 ; 0000-0002-0942-688X ; 0000-0002-0051-3661 ; 0000-0001-5030-7412 ; 000000020942688X ; 0000000237293148 ; 0000000284172488 ; 0000000150307412 ; 0000000200513661</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC9894257/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC9894257/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,727,780,784,885,27924,27925,53791,53793</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/36454748$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/servlets/purl/1974386$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Hou, Dong</creatorcontrib><creatorcontrib>Han, Jiaxiu</creatorcontrib><creatorcontrib>Geng, Chenxi</creatorcontrib><creatorcontrib>Xu, Zhengrui</creatorcontrib><creatorcontrib>AlMarzooqi, Modhi M</creatorcontrib><creatorcontrib>Zhang, Jin</creatorcontrib><creatorcontrib>Yang, Zhijie</creatorcontrib><creatorcontrib>Min, Jungki</creatorcontrib><creatorcontrib>Xiao, Xianghui</creatorcontrib><creatorcontrib>Borkiewicz, Olaf</creatorcontrib><creatorcontrib>Wiaderek, Kamila</creatorcontrib><creatorcontrib>Liu, Yijin</creatorcontrib><creatorcontrib>Zhao, Kejie</creatorcontrib><creatorcontrib>Lin, Feng</creatorcontrib><creatorcontrib>Argonne National Laboratory (ANL), Argonne, IL (United States)</creatorcontrib><creatorcontrib>SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)</creatorcontrib><creatorcontrib>Brookhaven National Laboratory (BNL), Upton, NY (United States)</creatorcontrib><title>Surface coating by mechanofusion modulates bulk charging pathways and battery performance of Ni-rich layered cathodes</title><title>Proceedings of the National Academy of Sciences - PNAS</title><addtitle>Proc Natl Acad Sci U S A</addtitle><description>Ni-rich layered oxides as high-capacity battery cathodes suffer from degradation at high voltages. We utilize a dry surface modification method, mechanofusion (MF), to achieve enhanced battery stability. The simplicity, high yield, and flexibility make it cost-effective and highly attractive for processing at the industrial scale. The underlying mechanisms responsible for performance improvement are unveiled by a systematic study combining multiple probes, e.g., 3D nano-tomography, spectroscopic imaging, in situ synchrotron diffraction, and finite element analysis (FEA). MF affects the bulk crystallography by introducing partially disordered structure, microstrain, and local lattice variation. Furthermore, the crack initiation and propagation pattern during delithiation are regulated and the overall mechanical fracture is reduced after such surface coating. We validate that MF can alter the bulk charging pathways. Such a synergic effect between surface modification and bulk charge distribution is fundamentally important for designing next-generation battery cathode materials.</description><subject>Batteries</subject><subject>Cathodes</subject><subject>Charge distribution</subject><subject>charge heterogeneity</subject><subject>Charging</subject><subject>coating</subject><subject>Crack initiation</subject><subject>Crack propagation</subject><subject>Crystallography</subject><subject>Electrode materials</subject><subject>ENERGY STORAGE</subject><subject>Finite element method</subject><subject>in situ XRD</subject><subject>Microstrain</subject><subject>Physical Sciences</subject><subject>rechargeable batteries</subject><subject>Synchrotrons</subject><subject>tomography</subject><issn>0027-8424</issn><issn>1091-6490</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNpdkc1v1DAQxS0EotuFMzdkwYVLWtuxE_uChCooSBUcgLM1azu7LokdbAeU_x6vtpSP0xzmN2_mzUPoGSUXlPTt5RwgXzBGmSSMUvUAbShRtOm4Ig_RhhDWN5IzfobOc74lhCghyWN01nZc8J7LDVo-L2kA47CJUHzY492KJ2cOEOKwZB8DnqJdRigu490yfsO1lfZHcIZy-AlrxhAs3kEpLq14dmmIaYJQFeOAP_omeXPAI6wuOYtNnYnW5Sfo0QBjdk_v6hZ9fff2y9X75ubT9YerNzeNEZSXRnY9I1RYa8F0jKjWmWqBCamIIHxw0AEoIgfFWtZXQ63rJBeya6W1PZXQbtHrk-687CZnjQslwajn5CdIq47g9b-d4A96H39oJRVnoq8CL04CMRevs_Gl_sbEEJwpmqqet3XbFr2625Li98XloiefjRtHCC4uWbOe865e1tGKvvwPvY1LCvUHlRKCimq4rdTliTIp5pzccH8xJfqYuz7mrv_kXiee_230nv8ddPsLZfqqTg</recordid><startdate>20221206</startdate><enddate>20221206</enddate><creator>Hou, Dong</creator><creator>Han, Jiaxiu</creator><creator>Geng, Chenxi</creator><creator>Xu, Zhengrui</creator><creator>AlMarzooqi, Modhi M</creator><creator>Zhang, Jin</creator><creator>Yang, Zhijie</creator><creator>Min, Jungki</creator><creator>Xiao, Xianghui</creator><creator>Borkiewicz, Olaf</creator><creator>Wiaderek, Kamila</creator><creator>Liu, Yijin</creator><creator>Zhao, Kejie</creator><creator>Lin, Feng</creator><general>National Academy of Sciences</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QG</scope><scope>7QL</scope><scope>7QP</scope><scope>7QR</scope><scope>7SN</scope><scope>7SS</scope><scope>7T5</scope><scope>7TK</scope><scope>7TM</scope><scope>7TO</scope><scope>7U9</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>H94</scope><scope>M7N</scope><scope>P64</scope><scope>RC3</scope><scope>7X8</scope><scope>OIOZB</scope><scope>OTOTI</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0002-3729-3148</orcidid><orcidid>https://orcid.org/0000-0002-8417-2488</orcidid><orcidid>https://orcid.org/0000-0002-0942-688X</orcidid><orcidid>https://orcid.org/0000-0002-0051-3661</orcidid><orcidid>https://orcid.org/0000-0001-5030-7412</orcidid><orcidid>https://orcid.org/000000020942688X</orcidid><orcidid>https://orcid.org/0000000237293148</orcidid><orcidid>https://orcid.org/0000000284172488</orcidid><orcidid>https://orcid.org/0000000150307412</orcidid><orcidid>https://orcid.org/0000000200513661</orcidid></search><sort><creationdate>20221206</creationdate><title>Surface coating by mechanofusion modulates bulk charging pathways and battery performance of Ni-rich layered cathodes</title><author>Hou, Dong ; 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We utilize a dry surface modification method, mechanofusion (MF), to achieve enhanced battery stability. The simplicity, high yield, and flexibility make it cost-effective and highly attractive for processing at the industrial scale. The underlying mechanisms responsible for performance improvement are unveiled by a systematic study combining multiple probes, e.g., 3D nano-tomography, spectroscopic imaging, in situ synchrotron diffraction, and finite element analysis (FEA). MF affects the bulk crystallography by introducing partially disordered structure, microstrain, and local lattice variation. Furthermore, the crack initiation and propagation pattern during delithiation are regulated and the overall mechanical fracture is reduced after such surface coating. We validate that MF can alter the bulk charging pathways. Such a synergic effect between surface modification and bulk charge distribution is fundamentally important for designing next-generation battery cathode materials.</abstract><cop>United States</cop><pub>National Academy of Sciences</pub><pmid>36454748</pmid><doi>10.1073/pnas.2212802119</doi><orcidid>https://orcid.org/0000-0002-3729-3148</orcidid><orcidid>https://orcid.org/0000-0002-8417-2488</orcidid><orcidid>https://orcid.org/0000-0002-0942-688X</orcidid><orcidid>https://orcid.org/0000-0002-0051-3661</orcidid><orcidid>https://orcid.org/0000-0001-5030-7412</orcidid><orcidid>https://orcid.org/000000020942688X</orcidid><orcidid>https://orcid.org/0000000237293148</orcidid><orcidid>https://orcid.org/0000000284172488</orcidid><orcidid>https://orcid.org/0000000150307412</orcidid><orcidid>https://orcid.org/0000000200513661</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | Batteries Cathodes Charge distribution charge heterogeneity Charging coating Crack initiation Crack propagation Crystallography Electrode materials ENERGY STORAGE Finite element method in situ XRD Microstrain Physical Sciences rechargeable batteries Synchrotrons tomography |
| title | Surface coating by mechanofusion modulates bulk charging pathways and battery performance of Ni-rich layered cathodes |
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