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Impact of temperature on short-range charge ordering in LiFePO4/FePO4
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-7596-9866
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0003-3570-0050
Rhein Westfal TH Aachen, Inst Phys Chem, D-52074 Aachen, Germany..
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-8019-2801
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2024 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 109, no 14, article id 144103Article in journal (Refereed) Published
Abstract [en]

Energy is stored in a LiFePO4 battery electrode through the intercalation of Li. As Li incorporate into the crystal lattice of Fe⁡(III)⁢PO4, electrons reduce Fe(III) into Fe(II). The interactions of Li and its vacant site (Va) with these localized electrons (holes), so-called polarons, cause phase separation during battery operation. These fundamental interactions are however difficult to quantify using standard electronic structure calculations. In this paper, we utilize DFT+𝑈 with occupation matrix control to compute interaction energies at varying Li-Fe(II) and Va-Fe(III) pair separations. The increased energy with separation warrants the use of an electrostatic description. The DFT+𝑈 data are fitted to a Coulombic potential with two-body corrections and used in a Monte Carlo scheme. The coordination of the species determines their short-range ordering, showing that the Li and Va create chains bridged by their associated polarons which dissociate into dimers at higher temperatures. This dissociation happens at higher temperatures for Va than for Li, indicating a more pronounced clustering behavior during the formation of FePO4. Notably, a significant amount of uncoordinated Li exists at elevated temperatures, challenging the simplified picture of complete Li-Fe(II) pairing.

Place, publisher, year, edition, pages
American Physical Society, 2024. Vol. 109, no 14, article id 144103
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Condensed Matter Physics Physical Chemistry Theoretical Chemistry
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URN: urn:nbn:se:uu:diva-530449DOI: 10.1103/PhysRevB.109.144103ISI: 001229771600002OAI: oai:DiVA.org:uu-530449DiVA, id: diva2:1865897
Funder
EU, Horizon 2020, 957189StandUpSwedish Research Council, 2022-06725eSSENCE - An eScience CollaborationNational Academic Infrastructure for Supercomputing in Sweden (NAISS)Available from: 2024-06-05 Created: 2024-06-05 Last updated: 2024-06-05Bibliographically approved

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Hammadi, SouzanKullgren, JollaBrandell, DanielBroqvist, Peter

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