Elucidating the sodiation mechanism in hard carbon by operando raman spectroscopy

Research output: Contribution to journalArticlepeer-review

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Elucidating the sodiation mechanism in hard carbon by operando raman spectroscopy. / Weaving, Julia S.; Lim, Alvin; Millichamp, Jason; Neville, Tobias P.; Ledwoch, Daniela; Kendrick, Emma; McMillan, Paul F.; Shearing, Paul R.; Howard, Christopher A.; Brett, Dan J.L.

In: ACS Applied Energy Materials, Vol. 3, No. 8, 24.08.2020, p. 7474-7484.

Research output: Contribution to journalArticlepeer-review

Harvard

Weaving, JS, Lim, A, Millichamp, J, Neville, TP, Ledwoch, D, Kendrick, E, McMillan, PF, Shearing, PR, Howard, CA & Brett, DJL 2020, 'Elucidating the sodiation mechanism in hard carbon by operando raman spectroscopy', ACS Applied Energy Materials, vol. 3, no. 8, pp. 7474-7484. https://doi.org/10.1021/acsaem.0c00867

APA

Weaving, J. S., Lim, A., Millichamp, J., Neville, T. P., Ledwoch, D., Kendrick, E., McMillan, P. F., Shearing, P. R., Howard, C. A., & Brett, D. J. L. (2020). Elucidating the sodiation mechanism in hard carbon by operando raman spectroscopy. ACS Applied Energy Materials, 3(8), 7474-7484. https://doi.org/10.1021/acsaem.0c00867

Vancouver

Author

Weaving, Julia S. ; Lim, Alvin ; Millichamp, Jason ; Neville, Tobias P. ; Ledwoch, Daniela ; Kendrick, Emma ; McMillan, Paul F. ; Shearing, Paul R. ; Howard, Christopher A. ; Brett, Dan J.L. / Elucidating the sodiation mechanism in hard carbon by operando raman spectroscopy. In: ACS Applied Energy Materials. 2020 ; Vol. 3, No. 8. pp. 7474-7484.

Bibtex

@article{8b8b6548d3e74da6a4fe0b0186a57fca,
title = "Elucidating the sodiation mechanism in hard carbon by operando raman spectroscopy",
abstract = "Operando microbeam Raman spectroscopy is used to map the changes in hard carbon during sodiation and desodiation in unprecedented detail, elucidating several important and unresolved aspects of the sodiation mechanism. On sodiation a substantial, reversible decrease in G-peak energy is observed, which corresponds directly to the sloping part of the voltage profile and we argue can only be due to steady intercalation of sodium between the turbostratic layers of the hard carbon. The corresponding reversibility of the D-peak energy change is consistent with intercalation rather than representing a permanent increase in disorder. No change in energy of the graphitic phonons occurs over the low-voltage plateau, indicating that intercalation saturates before sodium clusters form in micropores in this region. At the start of the initial sodiation there is no change in G- and D-peak energy as the solid electrolyte interphase (SEI) forms. After SEI formation, the background slope of the spectra increases irreversibly due to fluorescence. The importance of in situ/operando experiments over ex situ studies is demonstrated; washing the samples or air exposure causes the G- and D-peaks to revert back to their original states because of SEI removal and sodium deintercalation and confirms no permanent damage to the carbon structure.",
keywords = "Energy storage, Hard carbon, Operando Raman spectroscopy, Sodiation mechanism, Sodium-ion batteries",
author = "Weaving, {Julia S.} and Alvin Lim and Jason Millichamp and Neville, {Tobias P.} and Daniela Ledwoch and Emma Kendrick and McMillan, {Paul F.} and Shearing, {Paul R.} and Howard, {Christopher A.} and Brett, {Dan J.L.}",
year = "2020",
month = aug,
day = "24",
doi = "10.1021/acsaem.0c00867",
language = "English",
volume = "3",
pages = "7474--7484",
journal = "ACS Applied Energy Materials",
issn = "2574-0962",
publisher = "American Chemical Society",
number = "8",

}

RIS

TY - JOUR

T1 - Elucidating the sodiation mechanism in hard carbon by operando raman spectroscopy

AU - Weaving, Julia S.

AU - Lim, Alvin

AU - Millichamp, Jason

AU - Neville, Tobias P.

AU - Ledwoch, Daniela

AU - Kendrick, Emma

AU - McMillan, Paul F.

AU - Shearing, Paul R.

AU - Howard, Christopher A.

AU - Brett, Dan J.L.

PY - 2020/8/24

Y1 - 2020/8/24

N2 - Operando microbeam Raman spectroscopy is used to map the changes in hard carbon during sodiation and desodiation in unprecedented detail, elucidating several important and unresolved aspects of the sodiation mechanism. On sodiation a substantial, reversible decrease in G-peak energy is observed, which corresponds directly to the sloping part of the voltage profile and we argue can only be due to steady intercalation of sodium between the turbostratic layers of the hard carbon. The corresponding reversibility of the D-peak energy change is consistent with intercalation rather than representing a permanent increase in disorder. No change in energy of the graphitic phonons occurs over the low-voltage plateau, indicating that intercalation saturates before sodium clusters form in micropores in this region. At the start of the initial sodiation there is no change in G- and D-peak energy as the solid electrolyte interphase (SEI) forms. After SEI formation, the background slope of the spectra increases irreversibly due to fluorescence. The importance of in situ/operando experiments over ex situ studies is demonstrated; washing the samples or air exposure causes the G- and D-peaks to revert back to their original states because of SEI removal and sodium deintercalation and confirms no permanent damage to the carbon structure.

AB - Operando microbeam Raman spectroscopy is used to map the changes in hard carbon during sodiation and desodiation in unprecedented detail, elucidating several important and unresolved aspects of the sodiation mechanism. On sodiation a substantial, reversible decrease in G-peak energy is observed, which corresponds directly to the sloping part of the voltage profile and we argue can only be due to steady intercalation of sodium between the turbostratic layers of the hard carbon. The corresponding reversibility of the D-peak energy change is consistent with intercalation rather than representing a permanent increase in disorder. No change in energy of the graphitic phonons occurs over the low-voltage plateau, indicating that intercalation saturates before sodium clusters form in micropores in this region. At the start of the initial sodiation there is no change in G- and D-peak energy as the solid electrolyte interphase (SEI) forms. After SEI formation, the background slope of the spectra increases irreversibly due to fluorescence. The importance of in situ/operando experiments over ex situ studies is demonstrated; washing the samples or air exposure causes the G- and D-peaks to revert back to their original states because of SEI removal and sodium deintercalation and confirms no permanent damage to the carbon structure.

KW - Energy storage

KW - Hard carbon

KW - Operando Raman spectroscopy

KW - Sodiation mechanism

KW - Sodium-ion batteries

UR - http://www.scopus.com/inward/record.url?scp=85090941273&partnerID=8YFLogxK

U2 - 10.1021/acsaem.0c00867

DO - 10.1021/acsaem.0c00867

M3 - Article

AN - SCOPUS:85090941273

VL - 3

SP - 7474

EP - 7484

JO - ACS Applied Energy Materials

JF - ACS Applied Energy Materials

SN - 2574-0962

IS - 8

ER -