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Full Energy Range Resonant Inelastic X-Ray Scattering of O2 and CO2: Direct Comparison with Oxygen Redox State in Batteries

preprint
submitted on 08.12.2019 and posted on 16.12.2019 by Zengqing Zhuo, Yi-Sheng Liu, Jinghua Guo, Yi-de Chuang, Feng Pan, Wanli Yang
The varying oxygen state plays key roles in the performance and stability of various electrochemical systems. However, the nature of the non-divalent state remains elusive with speculations under active debates. A direct comparison between these unconventional states on their full oxygen spectroscopic profile is critical but remains missing. Here, high-efficiency full energy range O-K mapping of resonant inelastic x-ray scattering (mRIXS) was collected from O2 (O0) and CO2 (O2-) gas molecules. The results are compared directly with Li2O2 (O1-) and more importantly, the oxidized oxygen (On-, 0-n-2) state in representative Na-ion and Li-ion battery electrodes. All the mRIXS features of O2 and CO2 are interpreted, and we focus on the contrasts of two characteristic features among all oxidized oxygen species, especially on the striking 523.7 eV emission feature. The full mRIXS profile reveals that oxygen redox states in batteries have distinct distributions along the excitation energy compared with Li2O2 and O2. This work provides not only the first full range mRIXS results of O2 and CO2, but also the direct comparison of four different oxygen states, i.e., O2-, O1-, On-(0-n-2), and O0. Our results indicate that the nature of the oxidized oxygen state in oxide electrodes is beyond a simple molecular configuration of either peroxide or O2.

Funding

US DOE contract no. DE-AC02-05CH11231

LDRD of Lawrence Berkeley National Laboratory

Guangdong Key-lab Project No. 2017B0303010130

Shenzhen Science and Technology Research Grant No. ZDSYS20170728102618

History

Email Address of Submitting Author

WLYang@lbl.gov

Institution

Lawrence Berkeley National Laboratory

Country

United States

ORCID For Submitting Author

0000-0003-0666-8063

Declaration of Conflict of Interest

None

Exports