Electron paramagnetic resonance as a tool to determine the sodium charge storage mechanism of hard carbon.

Autor: Wang B; Department of Chemistry, Lancaster University, Lancaster, LA1 4YB, UK.; The Faraday Institution, Harwell Science and Innovation Campus, Quad One, Didcot, OX11 0RA, UK., Fitzpatrick JR; Department of Chemistry, Lancaster University, Lancaster, LA1 4YB, UK.; The Faraday Institution, Harwell Science and Innovation Campus, Quad One, Didcot, OX11 0RA, UK.; Department of Chemistry, Molecular Sciences Research Hub, White City Campus, Imperial College London, London, W12 0BZ, UK., Brookfield A; The National Research Facility for Electron Paramagnetic Resonance, Photon Science Institute, University of Manchester, Oxford Road, Manchester, M13 9PL, UK., Fielding AJ; Centre for Natural Products Discovery, School of Pharmacy and Biomolecular Sciences, Liverpool John Moore University, Byrom Street, Liverpool, L3 3AF, UK., Reynolds E; ISIS Neutron and Muon Spallation Source, STFC Rutherford Appleton Laboratory, Harwell, Oxford, OX11 0QX, UK., Entwistle J; Department of Chemistry, Lancaster University, Lancaster, LA1 4YB, UK., Tong J; Department of Chemistry, University of Manchester, Oxford Road, Manchester, M13 9PL, UK., Spencer BF; Department of Materials, University of Manchester, Oxford Road, Manchester, M13 9PL, UK., Baldock S; Department of Chemistry, Lancaster University, Lancaster, LA1 4YB, UK., Hunter K; Deregallera Ltd, Unit 2 De Clare Court, Pontygwindy Industrial Estate, Caerphilly, Wales, CF83 3HU, UK., Kavanagh CM; Deregallera Ltd, Unit 2 De Clare Court, Pontygwindy Industrial Estate, Caerphilly, Wales, CF83 3HU, UK., Tapia-Ruiz N; Department of Chemistry, Lancaster University, Lancaster, LA1 4YB, UK. n.tapia-ruiz@imperial.ac.uk.; The Faraday Institution, Harwell Science and Innovation Campus, Quad One, Didcot, OX11 0RA, UK. n.tapia-ruiz@imperial.ac.uk.; Department of Chemistry, Molecular Sciences Research Hub, White City Campus, Imperial College London, London, W12 0BZ, UK. n.tapia-ruiz@imperial.ac.uk.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2024 Apr 08; Vol. 15 (1), pp. 3013. Date of Electronic Publication: 2024 Apr 08.
DOI: 10.1038/s41467-024-45460-3
Abstrakt: Hard carbon is a promising negative electrode material for rechargeable sodium-ion batteries due to the ready availability of their precursors and high reversible charge storage. The reaction mechanisms that drive the sodiation properties in hard carbons and subsequent electrochemical performance are strictly linked to the characteristic slope and plateau regions observed in the voltage profile of these materials. This work shows that electron paramagnetic resonance (EPR) spectroscopy is a powerful and fast diagnostic tool to predict the extent of the charge stored in the slope and plateau regions during galvanostatic tests in hard carbon materials. EPR lineshape simulation and temperature-dependent measurements help to separate the nature of the spins in mechanochemically modified hard carbon materials synthesised at different temperatures. This proves relationships between structure modification and electrochemical signatures in the galvanostatic curves to obtain information on their sodium storage mechanism. Furthermore, through ex situ EPR studies we study the evolution of these EPR signals at different states of charge to further elucidate the storage mechanisms in these carbons. Finally, we discuss the interrelationship between EPR spectroscopy data of the hard carbon samples studied and their corresponding charging storage mechanism.
(© 2024. The Author(s).)
Databáze: MEDLINE
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