Distinction between Intrinsic and X-ray-Induced Oxidized Oxygen States in Li-Rich 3d Layered Oxides and LiAlO2

Zachary W. Lebens-Higgins, Julija Vinckeviciute, Jinpeng Wu, Nicholas V. Faenza, Yixuan Li, Shawn Sallis, Nathalie Pereira, Ying Shirley Meng, Glenn Amatucci, Anton Van Der Ven, Wanli Yang, Louis F.J. Piper

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Resonant inelastic X-ray scattering (RIXS) at the O K-edge is considered a prime technique to identify bulk oxidized oxygen formation, but its fundamental interpretation is not straightforward. In this study, we intentionally induce RIXS signatures of oxidized oxygen upon beam exposure in LiAlO2 polymorphs that are easily distinguished because of their wide band gaps. After careful consideration of beam exposure effects on Li[Li0.144Ni0.136Mn0.544Co0.136]O2 (LR-NMC), we conclude that oxidized oxygen features are inherent at high states of charge and are lost upon aggressive beam exposure. The extracted oxidized oxygen line shapes from our X-ray irradiation studies for both LiAlO2 (induced) and LR-NMC (inherent) are found to have an additional oxidized oxygen RIXS feature not observed in O2 gas studies. This study highlights the unique insight of O K-edge RIXS into determining the nature and stability of oxidized oxygen states.

Original languageEnglish (US)
Pages (from-to)13201-13207
Number of pages7
JournalJournal of Physical Chemistry C
Volume123
Issue number21
DOIs
StatePublished - May 30 2019

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Oxides
Inelastic scattering
Oxygen
X ray scattering
X rays
oxides
oxygen
x rays
scattering
Polymorphism
line shape
Energy gap
Gases
signatures
Irradiation
broadband
irradiation
gases

All Science Journal Classification (ASJC) codes

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

Cite this

Lebens-Higgins, Z. W., Vinckeviciute, J., Wu, J., Faenza, N. V., Li, Y., Sallis, S., ... Piper, L. F. J. (2019). Distinction between Intrinsic and X-ray-Induced Oxidized Oxygen States in Li-Rich 3d Layered Oxides and LiAlO2. Journal of Physical Chemistry C, 123(21), 13201-13207. https://doi.org/10.1021/acs.jpcc.9b01298
Lebens-Higgins, Zachary W. ; Vinckeviciute, Julija ; Wu, Jinpeng ; Faenza, Nicholas V. ; Li, Yixuan ; Sallis, Shawn ; Pereira, Nathalie ; Meng, Ying Shirley ; Amatucci, Glenn ; Der Ven, Anton Van ; Yang, Wanli ; Piper, Louis F.J. / Distinction between Intrinsic and X-ray-Induced Oxidized Oxygen States in Li-Rich 3d Layered Oxides and LiAlO2. In: Journal of Physical Chemistry C. 2019 ; Vol. 123, No. 21. pp. 13201-13207.
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abstract = "Resonant inelastic X-ray scattering (RIXS) at the O K-edge is considered a prime technique to identify bulk oxidized oxygen formation, but its fundamental interpretation is not straightforward. In this study, we intentionally induce RIXS signatures of oxidized oxygen upon beam exposure in LiAlO2 polymorphs that are easily distinguished because of their wide band gaps. After careful consideration of beam exposure effects on Li[Li0.144Ni0.136Mn0.544Co0.136]O2 (LR-NMC), we conclude that oxidized oxygen features are inherent at high states of charge and are lost upon aggressive beam exposure. The extracted oxidized oxygen line shapes from our X-ray irradiation studies for both LiAlO2 (induced) and LR-NMC (inherent) are found to have an additional oxidized oxygen RIXS feature not observed in O2 gas studies. This study highlights the unique insight of O K-edge RIXS into determining the nature and stability of oxidized oxygen states.",
author = "Lebens-Higgins, {Zachary W.} and Julija Vinckeviciute and Jinpeng Wu and Faenza, {Nicholas V.} and Yixuan Li and Shawn Sallis and Nathalie Pereira and Meng, {Ying Shirley} and Glenn Amatucci and {Der Ven}, {Anton Van} and Wanli Yang and Piper, {Louis F.J.}",
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Lebens-Higgins, ZW, Vinckeviciute, J, Wu, J, Faenza, NV, Li, Y, Sallis, S, Pereira, N, Meng, YS, Amatucci, G, Der Ven, AV, Yang, W & Piper, LFJ 2019, 'Distinction between Intrinsic and X-ray-Induced Oxidized Oxygen States in Li-Rich 3d Layered Oxides and LiAlO2', Journal of Physical Chemistry C, vol. 123, no. 21, pp. 13201-13207. https://doi.org/10.1021/acs.jpcc.9b01298

Distinction between Intrinsic and X-ray-Induced Oxidized Oxygen States in Li-Rich 3d Layered Oxides and LiAlO2. / Lebens-Higgins, Zachary W.; Vinckeviciute, Julija; Wu, Jinpeng; Faenza, Nicholas V.; Li, Yixuan; Sallis, Shawn; Pereira, Nathalie; Meng, Ying Shirley; Amatucci, Glenn; Der Ven, Anton Van; Yang, Wanli; Piper, Louis F.J.

In: Journal of Physical Chemistry C, Vol. 123, No. 21, 30.05.2019, p. 13201-13207.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Distinction between Intrinsic and X-ray-Induced Oxidized Oxygen States in Li-Rich 3d Layered Oxides and LiAlO2

AU - Lebens-Higgins, Zachary W.

AU - Vinckeviciute, Julija

AU - Wu, Jinpeng

AU - Faenza, Nicholas V.

AU - Li, Yixuan

AU - Sallis, Shawn

AU - Pereira, Nathalie

AU - Meng, Ying Shirley

AU - Amatucci, Glenn

AU - Der Ven, Anton Van

AU - Yang, Wanli

AU - Piper, Louis F.J.

PY - 2019/5/30

Y1 - 2019/5/30

N2 - Resonant inelastic X-ray scattering (RIXS) at the O K-edge is considered a prime technique to identify bulk oxidized oxygen formation, but its fundamental interpretation is not straightforward. In this study, we intentionally induce RIXS signatures of oxidized oxygen upon beam exposure in LiAlO2 polymorphs that are easily distinguished because of their wide band gaps. After careful consideration of beam exposure effects on Li[Li0.144Ni0.136Mn0.544Co0.136]O2 (LR-NMC), we conclude that oxidized oxygen features are inherent at high states of charge and are lost upon aggressive beam exposure. The extracted oxidized oxygen line shapes from our X-ray irradiation studies for both LiAlO2 (induced) and LR-NMC (inherent) are found to have an additional oxidized oxygen RIXS feature not observed in O2 gas studies. This study highlights the unique insight of O K-edge RIXS into determining the nature and stability of oxidized oxygen states.

AB - Resonant inelastic X-ray scattering (RIXS) at the O K-edge is considered a prime technique to identify bulk oxidized oxygen formation, but its fundamental interpretation is not straightforward. In this study, we intentionally induce RIXS signatures of oxidized oxygen upon beam exposure in LiAlO2 polymorphs that are easily distinguished because of their wide band gaps. After careful consideration of beam exposure effects on Li[Li0.144Ni0.136Mn0.544Co0.136]O2 (LR-NMC), we conclude that oxidized oxygen features are inherent at high states of charge and are lost upon aggressive beam exposure. The extracted oxidized oxygen line shapes from our X-ray irradiation studies for both LiAlO2 (induced) and LR-NMC (inherent) are found to have an additional oxidized oxygen RIXS feature not observed in O2 gas studies. This study highlights the unique insight of O K-edge RIXS into determining the nature and stability of oxidized oxygen states.

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DO - 10.1021/acs.jpcc.9b01298

M3 - Article

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SP - 13201

EP - 13207

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

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ER -