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Phonon assisted ion diffusion in electrochemically cycled NaxCoO2
KTH, School of Engineering Sciences (SCI), Applied Physics. Department of Physics and Astronomy, Uppsala University, Box 516, SE 75120, Uppsala, Sweden, Box 516, SE; Physik-Institut, Universität Zürich, Winterthurerstrasse 190, CH 8057, Zürich, Switzerland.ORCID iD: 0000-0001-8879-7875
KTH, School of Engineering Sciences (SCI), Applied Physics.ORCID iD: 0000-0002-1129-9234
Department of Chemistry, Stockholm University, SE-10691 Stockholm, Sweden; PSI Center for Neutron and Muon Sciences, 5232 Villigen PSI, Switzerland.
Muon Science Laboratory, IMSS, KEK, Tokai, Ibaraki 319-1112, Japan.
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2025 (English)In: Materials Today Energy, ISSN 2468-6069, Vol. 54, article id 102072Article in journal (Refereed) Published
Abstract [en]

Understanding ion diffusion mechanisms in layered materials is critical for advancing next-generation battery technologies. Using the well-characterized NaxCoO2 (NCO) system as a model platform, we investigated the temperature-dependent diffusion properties across a broad compositional range (x=0.33−0.89) using muon spin relaxation (μ+SR). Unexpected low-temperature internal magnetic field fluctuations were observed, systematically varying with Na content and appearing well before the onset of long-range diffusion. These fluctuations are attributed to phonon-assisted local Na motion, as suggested by a systematic increase in A with x, concurrent with a decreasing activation energy. The diffusion coefficient was calculated based on the crystal structure using a tailored diffusion model accounting for two inequivalent Na sites, yielding values consistent with those found in other layered battery materials. This work highlights the crucial role of phonon-coupled diffusion mechanisms in enabling ion transport at the microscopic scale, providing new insights into ion dynamics in layered solid-state conductors and their relevance to sodium-ion battery technology.

Place, publisher, year, edition, pages
Elsevier BV , 2025. Vol. 54, article id 102072
Keywords [en]
Ion diffusion, Muon spin relaxation, NaCoO2, Phonons
National Category
Condensed Matter Physics Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-372461DOI: 10.1016/j.mtener.2025.102072Scopus ID: 2-s2.0-105019322693OAI: oai:DiVA.org:kth-372461DiVA, id: diva2:2012185
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Not duplicate with DiVA 1614499

QC 20251107

Available from: 2025-11-07 Created: 2025-11-07 Last updated: 2025-11-07Bibliographically approved

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Forslund, Ola K.Palm, RasmusZubayer, AntonSassa, YasmineMånsson, Martin

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