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Enhancing the performance of hard carbon for sodium-ion batteries by coating with silicon nitride/oxycarbide nanoparticles

Enhancing the performance of hard carbon for sodium-ion batteries by coating with silicon nitride/oxycarbide nanoparticles
Enhancing the performance of hard carbon for sodium-ion batteries by coating with silicon nitride/oxycarbide nanoparticles

A simple synthesis method to produce hard carbon decorated with silicon nitride or silicon oxycarbide nanoparticles was developed. Silicon tetrachloride is reacted with the hydroxide groups on cellulose (cotton wool) before carbonisation to form hard carbon. Use of a nitrogen or argon carbonisation atmosphere enables production of silicon nitride or oxycarbide coatings by carbothermal nitridation or reduction. This is the first time that a silicon nitride has been used in sodium-ion batteries, and it has a very high capacity. The incorporation of 7.9 wt% of silicon nitride produces an increase in the reversible (desodiation) capacity from 284 mA h g-1 for pure hard carbon to 351 mA h g-1 for the silicon nitride-hard carbon composite, at 50 mA g-1 in sodium half-cells. The associated silicon nitride capacity is estimated as 848 mA h g-1 when normalised by the mass of silicon nitride, ascribed to the good dispersion of silicon nitride nanoparticles on the hard carbon, and facile electrochemical reactions in the amorphous and non-stoichiometric silicon nitride. X-ray photoelectron spectroscopy (XPS) of the electrodes before and after cycling is used to elucidate the mechanism of sodium storage, involving formation of amorphous silicon, which then reacts with the electrolyte forming SiOx surface species.

2633-5409
7956-7966
Cheng, Hang
f3a86c10-c405-46da-b37d-28a37aa355aa
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Hector, Andrew L.
f19a8f31-b37f-4474-b32a-b7cf05b9f0e5
Cheng, Hang
f3a86c10-c405-46da-b37d-28a37aa355aa
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Hector, Andrew L.
f19a8f31-b37f-4474-b32a-b7cf05b9f0e5

Cheng, Hang, Garcia-Araez, Nuria and Hector, Andrew L. (2021) Enhancing the performance of hard carbon for sodium-ion batteries by coating with silicon nitride/oxycarbide nanoparticles. Materials Advances, 2 (24), 7956-7966. (doi:10.1039/D1MA00613D).

Record type: Article

Abstract

A simple synthesis method to produce hard carbon decorated with silicon nitride or silicon oxycarbide nanoparticles was developed. Silicon tetrachloride is reacted with the hydroxide groups on cellulose (cotton wool) before carbonisation to form hard carbon. Use of a nitrogen or argon carbonisation atmosphere enables production of silicon nitride or oxycarbide coatings by carbothermal nitridation or reduction. This is the first time that a silicon nitride has been used in sodium-ion batteries, and it has a very high capacity. The incorporation of 7.9 wt% of silicon nitride produces an increase in the reversible (desodiation) capacity from 284 mA h g-1 for pure hard carbon to 351 mA h g-1 for the silicon nitride-hard carbon composite, at 50 mA g-1 in sodium half-cells. The associated silicon nitride capacity is estimated as 848 mA h g-1 when normalised by the mass of silicon nitride, ascribed to the good dispersion of silicon nitride nanoparticles on the hard carbon, and facile electrochemical reactions in the amorphous and non-stoichiometric silicon nitride. X-ray photoelectron spectroscopy (XPS) of the electrodes before and after cycling is used to elucidate the mechanism of sodium storage, involving formation of amorphous silicon, which then reacts with the electrolyte forming SiOx surface species.

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Accepted/In Press date: 17 October 2021
e-pub ahead of print date: 19 October 2021
Published date: 21 December 2021
Additional Information: Funding Information: H. C. thanks the China Scholarship Council (CSC) and University of Southampton for support. N. G. A. thanks the EPSRC for an early career fellowship (EP/N024303/1). We acknowledge Harwell XPS for collecting the XPS data and Professor Andrea Russell for access to the Raman spectrometer. Raw data supporting this study are openly available from the University of Southampton repository at https://doi.org/10.5258/SOTON/ D2010. Publisher Copyright: © The Royal Society of Chemistry.

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Local EPrints ID: 452062
URI: http://eprints.soton.ac.uk/id/eprint/452062
ISSN: 2633-5409
PURE UUID: 79c2a5fb-866f-4eac-8ff6-9f27d927b0b0
ORCID for Nuria Garcia-Araez: ORCID iD orcid.org/0000-0001-9095-2379
ORCID for Andrew L. Hector: ORCID iD orcid.org/0000-0002-9964-2163

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Date deposited: 10 Nov 2021 17:33
Last modified: 17 Mar 2024 03:31

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Author: Hang Cheng

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