Elucidating sodium ion storage mechanisms in hard carbon anodes at the electronic level

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dc.contributor.authorXia, QBen_AU
dc.contributor.authorKo, CLen_AU
dc.contributor.authorCooper, ERen_AU
dc.contributor.authorGu, QFen_AU
dc.contributor.authorKnibbe, Ren_AU
dc.contributor.authorHarmer, JRen_AU
dc.date.accessioned2025-07-03T05:55:24Zen_AU
dc.date.available2025-07-03T05:55:24Zen_AU
dc.date.issued2025-02-17en_AU
dc.date.statistics2025-07en_AU
dc.description.abstractSodium‐ion batteries (SIBs) are a promising technology for advanced energy storage systems. Hard carbon (HC) is a commonly used SIB anode material; however, the Na ion storage mechanism in HC remains poorly understood and highly debated. Here, the paramagnetic species in HC during Na ion storage are systematically studied to elucidate the underlying mechanism at an electronic level using high‐resolution electron paramagnetic resonance (EPR) spectroscopy, complemented by in situ Raman spectroscopy, in situ synchrotron X‐ray diffraction, and density functional theory calculations. This investigation identifies and characterizes the coexistence of two distinct intercalation processes in HC: Na ion intercalation and Na+‐solvent co‐intercalation, which are active across both the sloping and plateau voltage regions. Additionally, in the sloping region, Na ions are also stored at in‐plane Stone‐Wales defect sites, which transition into a quasi‐metallic state and subsequently to metallic Na as Na ion intercalation progresses. This transformation is driven by charge redistribution within the graphene layers. These insights establish a direct paramagnetic‐electronic structure‐electrochemical property relationship in HC, providing new insights into the Na ion storage mechanism. Furthermore, this study highlights the unique capability of EPR spectroscopy in elucidating the charge storage mechanism in electrode materials. © 2025 The Author(s). Advanced Functional Materials published by Wiley-VCH GmbH. This is an open access article under the terms of th eCreative Commons Attribution-NonCommercial-NoDerivs License,which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are madeen_AU
dc.description.sponsorshipThis work was funded by the Australian Research Council through grants DP200102573, FT220100666, and LE230100048. The authors gratefully acknowledge the support provided by the Centre of Microscopy and Microanalysis (CMM) and the EPR facility at the The University of Queensland. The authors also thank the support received from the Powder Diffraction beamline at the Australian Synchrotron, part of ANSTO. The authors express their gratitude to Prof. Xiu Song (George) Zhao from The University of Queensland (now at Qingdao University) for his generous support in facilitating this work. Open access publishing facilitated by The University of Queensland, as part of the Wiley - The University of Queensland agreement via the Council of Australian University Librarians.en_AU
dc.identifier.articlenumber2421976en_AU
dc.identifier.citationXia, Q., Ko, C.-L., Cooper, E. R., Gu, Q., Knibbe, R., & Harmer, J. R. (2025). Elucidating sodium ion storage mechanisms in hard carbon anodes at the electronic level. Advanced Functional Materials, (Early view), 2421976. doi:10.1002/adfm.202421976en_AU
dc.identifier.issn1616-301Xen_AU
dc.identifier.issn1616-3028en_AU
dc.identifier.issue0en_AU
dc.identifier.journaltitleAdvanced Functional Materialsen_AU
dc.identifier.urihttps://doi.org/10.1002/adfm.202421976en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/16239en_AU
dc.identifier.volume0en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherWileyen_AU
dc.subjectLithium ion batteriesen_AU
dc.subjectEnergy storage systemsen_AU
dc.subjectEnergy storageen_AU
dc.subjectSodiumen_AU
dc.subjectCarbonen_AU
dc.subjectRaman spectroscopyen_AU
dc.subjectHigh energy physicsen_AU
dc.subjectAdsorptionen_AU
dc.titleElucidating sodium ion storage mechanisms in hard carbon anodes at the electronic levelen_AU
dc.typeJournal Articleen_AU
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