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Title: Electronic structure changes upon lithium intercalation into graphite – Insights from ex situ and operando x-ray Raman spectroscopy

Abstract

This study probes the electrochemical intercalation mechanism of Li into graphitic carbon using x-ray Raman spectroscopy (XRS), an inelastic x-ray scattering technique. Operando and high resolution spectra of electrochemically lithiated composite graphitic electrodes at discrete states of Li uptake (stages III, II and I) show gradually changing spectral features with Li intercalation, the end state agreeing well with chemically fully lithiated LiC 6 highly oriented pyrolytic graphite (HOPG). The two most dominant changes in the XRS spectrum of the C-K edge are the reduced intensity of the $$\pi$$* peak and shift the onset of the σ* states to lower energies upon full lithiation. The excellent instrumental energy resolution uncovered novel spectral features and, thus, electronic changes with varying lithium content. Thus, the general spectral changes with progressing Li intercalation agree well with our accompanying DFT calculations.

Authors:
 [1];  [2];  [2];  [2];  [3];  [4];  [4];  [5]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); European X-Ray Free-Electron Laser Facility, Schenefeld (Germany)
  2. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  3. European X-Ray Free-Electron Laser Facility, Schenefeld (Germany)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Illinois, Chicago, IL (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1502989
Grant/Contract Number:  
AC02-76SF00515; SC0001294
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Carbon
Additional Journal Information:
Journal Volume: 143; Journal Issue: C; Journal ID: ISSN 0008-6223
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Boesenberg, Ulrike, Sokaras, Dimosthenis, Nordlund, Dennis, Weng, Tsu-Chien, Gorelov, Evgeny, Richardson, Thomas J., Kostecki, Robert, and Cabana, Jordi. Electronic structure changes upon lithium intercalation into graphite – Insights from ex situ and operando x-ray Raman spectroscopy. United States: N. p., 2018. Web. doi:10.1016/j.carbon.2018.11.031.
Boesenberg, Ulrike, Sokaras, Dimosthenis, Nordlund, Dennis, Weng, Tsu-Chien, Gorelov, Evgeny, Richardson, Thomas J., Kostecki, Robert, & Cabana, Jordi. Electronic structure changes upon lithium intercalation into graphite – Insights from ex situ and operando x-ray Raman spectroscopy. United States. doi:10.1016/j.carbon.2018.11.031.
Boesenberg, Ulrike, Sokaras, Dimosthenis, Nordlund, Dennis, Weng, Tsu-Chien, Gorelov, Evgeny, Richardson, Thomas J., Kostecki, Robert, and Cabana, Jordi. Tue . "Electronic structure changes upon lithium intercalation into graphite – Insights from ex situ and operando x-ray Raman spectroscopy". United States. doi:10.1016/j.carbon.2018.11.031.
@article{osti_1502989,
title = {Electronic structure changes upon lithium intercalation into graphite – Insights from ex situ and operando x-ray Raman spectroscopy},
author = {Boesenberg, Ulrike and Sokaras, Dimosthenis and Nordlund, Dennis and Weng, Tsu-Chien and Gorelov, Evgeny and Richardson, Thomas J. and Kostecki, Robert and Cabana, Jordi},
abstractNote = {This study probes the electrochemical intercalation mechanism of Li into graphitic carbon using x-ray Raman spectroscopy (XRS), an inelastic x-ray scattering technique. Operando and high resolution spectra of electrochemically lithiated composite graphitic electrodes at discrete states of Li uptake (stages III, II and I) show gradually changing spectral features with Li intercalation, the end state agreeing well with chemically fully lithiated LiC6 highly oriented pyrolytic graphite (HOPG). The two most dominant changes in the XRS spectrum of the C-K edge are the reduced intensity of the $\pi$* peak and shift the onset of the σ* states to lower energies upon full lithiation. The excellent instrumental energy resolution uncovered novel spectral features and, thus, electronic changes with varying lithium content. Thus, the general spectral changes with progressing Li intercalation agree well with our accompanying DFT calculations.},
doi = {10.1016/j.carbon.2018.11.031},
journal = {Carbon},
issn = {0008-6223},
number = C,
volume = 143,
place = {United States},
year = {2018},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on November 13, 2019
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