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

Boesenberg, Ulrike; Sokaras, Dimosthenis; Nordlund, Dennis; Weng, Tsu-Chien; Gorelov, Evgeny; Richardson, Thomas J.; Kostecki, Robert; Cabana, Jordi

doi:10.1016/j.carbon.2018.11.031

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

Journal Article · Tue Nov 13 00:00:00 EST 2018 · Carbon

DOI:https://doi.org/10.1016/j.carbon.2018.11.031· OSTI ID:1502989

Boesenberg, Ulrike ^[1]; Sokaras, Dimosthenis ^[2]; Nordlund, Dennis ^[2]; Weng, Tsu-Chien ^[2]; Gorelov, Evgeny ^[3]; Richardson, Thomas J. ^[4]; Kostecki, Robert ^[4]; Cabana, Jordi ^[5]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); European X-Ray Free-Electron Laser Facility, Schenefeld (Germany)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
European X-Ray Free-Electron Laser Facility, Schenefeld (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Illinois, Chicago, IL (United States)

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.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; SC0001294

OSTI ID:: 1502989

Alternate ID(s):: OSTI ID: 1635847

Journal Information:: Carbon, Vol. 143, Issue C; ISSN 0008-6223

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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