Mechanistic insights into cathode-driven capacity degradation of NMC111/ graphite pouch cells under long-term cycling

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dc.contributor.authorAtes, Mehmet Nurullah
dc.contributor.authorZengin, Feyza
dc.contributor.authorWhba, Rawdah
dc.contributor.authorTunaboylu, Bahadir
dc.contributor.authorAydemir, Umut
dc.contributor.authorPeighambardoust, Naeimeh Sadat
dc.contributor.authorKarslioglu, Nergiz Gurbuz
dc.date.accessioned2026-04-04T13:35:08Z
dc.date.available2026-04-04T13:35:08Z
dc.date.issued2025
dc.departmentİnönü Üniversitesi
dc.description.abstractTo investigate long-term degradation, 2000 mAh NMC111/graphite (Gr) pouch cells were cycled 5500 times at a 1C rate. After cycling, the resulting degradation mechanisms were systematically analyzed. Structurally, X-ray diffraction (XRD) peak shifts (003, 108, 110) revealed Jahn-Teller (JT) distortion, evidenced by an increase in the c-lattice parameter. This led to the rise in internal resistance, consistent with scanning electron microscopy (SEM) images that revealed pronounced grain deformation on the cathode. Chemically, ex-situ X-ray absorption near-edge structure (XANES) spectroscopy revealed an increase in the valence states of Mn, Ni, and Co ions, indicating significant bulk changes that could potentially destabilize the oxygen lattice. X-ray absorption fine structure (XAFS) analysis further underscored the key role of weakening transition metal-oxygen (TM-O) bonds in driving this structural deformation. At the surface, X-ray photoelectron spectroscopy (XPS) confirmed the formation of a cathode-electrolyte interphase (CEI) comprising lithium fluoride (LiF), LixPFy, and organic carbonates. The progression of these surface reactions is a key contributor to impedance growth and capacity fade over long-term cycling.
dc.description.sponsorshipBogazici University Research Fund [19,862, 23B05SUP2, 50,028, 24BYOKADP1]; TUBITAK through the 2232 International Fellowship for Outstanding Researchers Program; Ministry of Development [2014K121080]; TUBITAK B IDEB National Ph.D. Scholarship Program [2211-A]
dc.description.sponsorshipThe authors sincerely thank the ROCK beamline team at SOLEIL Synchrotron (France) for their support during the Operando XAS measurements. They are grateful to the Turkish Energy, Nuclear and Mineral Research Agency (TENMAK) for providing travel support to S. Alt & imath;n and M.N. Ates for the experiments at SOLEIL. This project was financially supported by the Bogazici University Research Fund (Project No. 19,862, BOUN No. 23B05SUP2) , with additional financial and infrastructure support from the same fund (Project No. 50,028, BOUN No. 24BYOKADP1) . M.N. Ates sincerely acknowledges the prestigious support of TUBITAK through the 2232 International Fellowship for Outstanding Researchers Program. They also extend our gratitude to the Presidency of Strategy and Budget of Turkiye (formerly the Ministry of Development) for funding under Contract No. 2014K121080. Finally, Feyza Zengin gratefully acknowledges support from the TUBITAK B IDEB National Ph.D. Scholarship Program (2211-A) .
dc.identifier.doi10.1016/j.electacta.2025.147611
dc.identifier.issn0013-4686
dc.identifier.issn1873-3859
dc.identifier.orcid0000-0002-4786-897X
dc.identifier.orcid0000-0003-1804-5963
dc.identifier.scopus2-s2.0-105022198914
dc.identifier.scopusqualityQ1
dc.identifier.urihttps://doi.org/10.1016/j.electacta.2025.147611
dc.identifier.urihttps://hdl.handle.net/11616/109640
dc.identifier.volume543
dc.identifier.wosWOS:001606041400006
dc.identifier.wosqualityQ1
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.language.isoen
dc.publisherPergamon-Elsevier Science Ltd
dc.relation.ispartofElectrochimica Acta
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_WOS_20250329
dc.subjectNMC111
dc.subjectPouch cell
dc.subjectCathode-electrolyte interphase
dc.subjectCapacity fade
dc.subjectBatteries
dc.titleMechanistic insights into cathode-driven capacity degradation of NMC111/ graphite pouch cells under long-term cycling
dc.typeArticle

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