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

Wang, Bin and Fitzpatrick, Jack R. and Brookfield, Adam and Fielding, Alistair J. and Reynolds, Emily and Entwistle, Jake and Tong, Jincheng and Spencer, Ben F. and Baldock, Sara and Hunter, Katherine and Kavanagh, Christopher M. and Tapia-Ruiz, Nuria (2024) Electron paramagnetic resonance as a tool to determine the sodium charge storage mechanism of hard carbon. Nature Communications, 15 (1): 3013. ISSN 2041-1723

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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.

Item Type:
Journal Article
Journal or Publication Title:
Nature Communications
Uncontrolled Keywords:
/dk/atira/pure/subjectarea/asjc/1300
Subjects:
?? biochemistry, genetics and molecular biology(all)chemistry(all)physics and astronomy(all) ??
ID Code:
217915
Deposited By:
Deposited On:
15 Apr 2024 09:25
Refereed?:
Yes
Published?:
Published
Last Modified:
15 Apr 2024 09:25