Enhanced lithiation of doped 6H silicon carbide (0001) via high temperature vacuum growth of epitaxial graphene

Albert L. Lipson, Sudeshna Chattopadhyay, Hunter J. Karmel, Timothy T. Fister, Jonathan D. Emery, Vinayak P. Dravid, Michael M. Thackeray, Paul A. Fenter, Michael J. Bedzyk, Mark C Hersam

Research output: Contribution to journalArticle

18 Citations (Scopus)

Abstract

The electrochemical lithiation capacity of 6H silicon carbide (0001) is found to increase by over 1 order of magnitude following graphitization at 1350 °C in ultrahigh vacuum. Through several control experiments, this Li-ion capacity enhancement is correlated with SiC substrate doping and removal of the native oxide surface layer by thermal annealing, which renders both the bulk and surface electrically conductive. Characterization via multiple depth-resolved spectroscopies shows that lithium penetrates the activated SiC upon lithiation, the bulk lattice spacing does not appreciably change, and the surface structure remains largely intact. The electron energy-loss spectroscopy (EELS) extracted compositional ratio of Li to Si is approximately 1:1, which indicates an intrinsic bulk Li capacity in activated SiC of 670 mAh g -1. In addition, inelastic X-ray scattering spectra show changes in the Si chemical bonding configuration due to lithiation. X-ray scattering data show a decrease in the SiC Bragg peak intensity during lithiation, suggesting changes to the bulk crystallinity, whereas the emergence of a diffuse scattering feature suggests that lithiation is associated with the development of substrate defects. Overall, these results illustrate that the electrochemical capacity of a traditionally inert refractory material can be increased substantially via surface modification, thus suggesting a new strategy for improving the performance of next generation Li-ion battery electrodes.

Original languageEnglish
Pages (from-to)20949-20957
Number of pages9
JournalJournal of Physical Chemistry C
Volume116
Issue number39
DOIs
Publication statusPublished - Oct 4 2012

Fingerprint

Graphite
X ray scattering
Silicon carbide
silicon carbides
Graphene
graphene
Vacuum
vacuum
Inelastic scattering
Graphitization
Electron energy loss spectroscopy
Ultrahigh vacuum
Substrates
Lithium
Surface structure
Refractory materials
Oxides
Surface treatment
scattering
Doping (additives)

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

Enhanced lithiation of doped 6H silicon carbide (0001) via high temperature vacuum growth of epitaxial graphene. / Lipson, Albert L.; Chattopadhyay, Sudeshna; Karmel, Hunter J.; Fister, Timothy T.; Emery, Jonathan D.; Dravid, Vinayak P.; Thackeray, Michael M.; Fenter, Paul A.; Bedzyk, Michael J.; Hersam, Mark C.

In: Journal of Physical Chemistry C, Vol. 116, No. 39, 04.10.2012, p. 20949-20957.

Research output: Contribution to journalArticle

Lipson, AL, Chattopadhyay, S, Karmel, HJ, Fister, TT, Emery, JD, Dravid, VP, Thackeray, MM, Fenter, PA, Bedzyk, MJ & Hersam, MC 2012, 'Enhanced lithiation of doped 6H silicon carbide (0001) via high temperature vacuum growth of epitaxial graphene', Journal of Physical Chemistry C, vol. 116, no. 39, pp. 20949-20957. https://doi.org/10.1021/jp307220y
Lipson, Albert L. ; Chattopadhyay, Sudeshna ; Karmel, Hunter J. ; Fister, Timothy T. ; Emery, Jonathan D. ; Dravid, Vinayak P. ; Thackeray, Michael M. ; Fenter, Paul A. ; Bedzyk, Michael J. ; Hersam, Mark C. / Enhanced lithiation of doped 6H silicon carbide (0001) via high temperature vacuum growth of epitaxial graphene. In: Journal of Physical Chemistry C. 2012 ; Vol. 116, No. 39. pp. 20949-20957.
@article{9f8c4baa1d3943279e482bf0b73def84,
title = "Enhanced lithiation of doped 6H silicon carbide (0001) via high temperature vacuum growth of epitaxial graphene",
abstract = "The electrochemical lithiation capacity of 6H silicon carbide (0001) is found to increase by over 1 order of magnitude following graphitization at 1350 °C in ultrahigh vacuum. Through several control experiments, this Li-ion capacity enhancement is correlated with SiC substrate doping and removal of the native oxide surface layer by thermal annealing, which renders both the bulk and surface electrically conductive. Characterization via multiple depth-resolved spectroscopies shows that lithium penetrates the activated SiC upon lithiation, the bulk lattice spacing does not appreciably change, and the surface structure remains largely intact. The electron energy-loss spectroscopy (EELS) extracted compositional ratio of Li to Si is approximately 1:1, which indicates an intrinsic bulk Li capacity in activated SiC of 670 mAh g -1. In addition, inelastic X-ray scattering spectra show changes in the Si chemical bonding configuration due to lithiation. X-ray scattering data show a decrease in the SiC Bragg peak intensity during lithiation, suggesting changes to the bulk crystallinity, whereas the emergence of a diffuse scattering feature suggests that lithiation is associated with the development of substrate defects. Overall, these results illustrate that the electrochemical capacity of a traditionally inert refractory material can be increased substantially via surface modification, thus suggesting a new strategy for improving the performance of next generation Li-ion battery electrodes.",
author = "Lipson, {Albert L.} and Sudeshna Chattopadhyay and Karmel, {Hunter J.} and Fister, {Timothy T.} and Emery, {Jonathan D.} and Dravid, {Vinayak P.} and Thackeray, {Michael M.} and Fenter, {Paul A.} and Bedzyk, {Michael J.} and Hersam, {Mark C}",
year = "2012",
month = "10",
day = "4",
doi = "10.1021/jp307220y",
language = "English",
volume = "116",
pages = "20949--20957",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "39",

}

TY - JOUR

T1 - Enhanced lithiation of doped 6H silicon carbide (0001) via high temperature vacuum growth of epitaxial graphene

AU - Lipson, Albert L.

AU - Chattopadhyay, Sudeshna

AU - Karmel, Hunter J.

AU - Fister, Timothy T.

AU - Emery, Jonathan D.

AU - Dravid, Vinayak P.

AU - Thackeray, Michael M.

AU - Fenter, Paul A.

AU - Bedzyk, Michael J.

AU - Hersam, Mark C

PY - 2012/10/4

Y1 - 2012/10/4

N2 - The electrochemical lithiation capacity of 6H silicon carbide (0001) is found to increase by over 1 order of magnitude following graphitization at 1350 °C in ultrahigh vacuum. Through several control experiments, this Li-ion capacity enhancement is correlated with SiC substrate doping and removal of the native oxide surface layer by thermal annealing, which renders both the bulk and surface electrically conductive. Characterization via multiple depth-resolved spectroscopies shows that lithium penetrates the activated SiC upon lithiation, the bulk lattice spacing does not appreciably change, and the surface structure remains largely intact. The electron energy-loss spectroscopy (EELS) extracted compositional ratio of Li to Si is approximately 1:1, which indicates an intrinsic bulk Li capacity in activated SiC of 670 mAh g -1. In addition, inelastic X-ray scattering spectra show changes in the Si chemical bonding configuration due to lithiation. X-ray scattering data show a decrease in the SiC Bragg peak intensity during lithiation, suggesting changes to the bulk crystallinity, whereas the emergence of a diffuse scattering feature suggests that lithiation is associated with the development of substrate defects. Overall, these results illustrate that the electrochemical capacity of a traditionally inert refractory material can be increased substantially via surface modification, thus suggesting a new strategy for improving the performance of next generation Li-ion battery electrodes.

AB - The electrochemical lithiation capacity of 6H silicon carbide (0001) is found to increase by over 1 order of magnitude following graphitization at 1350 °C in ultrahigh vacuum. Through several control experiments, this Li-ion capacity enhancement is correlated with SiC substrate doping and removal of the native oxide surface layer by thermal annealing, which renders both the bulk and surface electrically conductive. Characterization via multiple depth-resolved spectroscopies shows that lithium penetrates the activated SiC upon lithiation, the bulk lattice spacing does not appreciably change, and the surface structure remains largely intact. The electron energy-loss spectroscopy (EELS) extracted compositional ratio of Li to Si is approximately 1:1, which indicates an intrinsic bulk Li capacity in activated SiC of 670 mAh g -1. In addition, inelastic X-ray scattering spectra show changes in the Si chemical bonding configuration due to lithiation. X-ray scattering data show a decrease in the SiC Bragg peak intensity during lithiation, suggesting changes to the bulk crystallinity, whereas the emergence of a diffuse scattering feature suggests that lithiation is associated with the development of substrate defects. Overall, these results illustrate that the electrochemical capacity of a traditionally inert refractory material can be increased substantially via surface modification, thus suggesting a new strategy for improving the performance of next generation Li-ion battery electrodes.

UR - http://www.scopus.com/inward/record.url?scp=84865133978&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84865133978&partnerID=8YFLogxK

U2 - 10.1021/jp307220y

DO - 10.1021/jp307220y

M3 - Article

VL - 116

SP - 20949

EP - 20957

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 39

ER -