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

Bin Wang, Jack R. Fitzpatrick, Adam Brookfield, Alistair J. Fielding, Emily Reynolds, Jake Entwistle, Jincheng Tong, Ben F. Spencer, Sara Baldock, Katherine Hunter, Christopher M. Kavanagh and Nuria Tapia-Ruiz ()
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Bin Wang: Lancaster University
Jack R. Fitzpatrick: Lancaster University
Adam Brookfield: University of Manchester
Alistair J. Fielding: Liverpool John Moore University
Emily Reynolds: ISIS Neutron and Muon Spallation Source, STFC Rutherford Appleton Laboratory, Harwell
Jake Entwistle: Lancaster University
Jincheng Tong: University of Manchester
Ben F. Spencer: University of Manchester
Sara Baldock: Lancaster University
Katherine Hunter: Deregallera Ltd, Unit 2 De Clare Court, Pontygwindy Industrial Estate
Christopher M. Kavanagh: Deregallera Ltd, Unit 2 De Clare Court, Pontygwindy Industrial Estate
Nuria Tapia-Ruiz: Lancaster University

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-45460-3

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