A revised mechanistic model for sodium insertion in hard carbons
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OA Location
Author(s)
Type
Journal Article
Abstract
Hard carbons have shown considerable promise as anodes for emerging sodium-ion battery technologies. Current understanding of sodium-storage behaviour in hard carbons attributes capacity to filling of graphitic interlayers and pores, and adsorption at defects, although there is still considerable debate regarding the voltages at which these mechanisms occur. Here, ex situ23Na solid-state NMR and total scattering studies on a systematically tuned series of hard carbons revealed the formation of increasingly metallic sodium clusters in direct correlation to the growing pore size, occurring only in samples which exhibited a low voltage plateau. Combining experimental results with DFT calculations, we propose a revised mechanistic model in which sodium ions store first simultaneously and continuously at defects, within interlayers and on pore surfaces. Once these higher energy binding sites are filled, pore filling occurs during the plateau region, where the densely confined sodium takes on a greater degree of metallicity.
Date Issued
2020-10-01
Date Acceptance
2020-07-31
Citation
Energy and Environmental Science, 2020, 13 (10), pp.3469-3479
ISSN
1754-5692
Publisher
Royal Society of Chemistry
Start Page
3469
End Page
3479
Journal / Book Title
Energy and Environmental Science
Volume
13
Issue
10
Copyright Statement
© The Royal Society of Chemistry 2020. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
License URL
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000579868500013&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Technology
Life Sciences & Biomedicine
Chemistry, Multidisciplinary
Energy & Fuels
Engineering, Chemical
Environmental Sciences
Chemistry
Engineering
Environmental Sciences & Ecology
INITIO MOLECULAR-DYNAMICS
TOTAL-ENERGY CALCULATIONS
ION STORAGE MECHANISM
AB-INITIO
ELECTRODE MATERIALS
NA
GRAPHENE
INSIGHTS
ANODE
LI
Publication Status
Published
Date Publish Online
2020-08-07