In-situ/operando X-ray absorption spectroscopic investigation of the electrode/electrolyte interface on the molecular scale

Kao, Li Cheng; Feng, Xuefei; Ha, Yang; Yang, Feipeng; Liu, Yi-Sheng; Hahn, Nathan T.; MacDougall, James; Chao, Weilun; Yang, Wanli; Zavadil, Kevin R.; Guo, Jinghua

doi:10.1016/j.susc.2020.121720

In-situ/operando X-ray absorption spectroscopic investigation of the electrode/electrolyte interface on the molecular scale

Journal Article · Sun Aug 23 00:00:00 EDT 2020 · Surface Science

DOI:https://doi.org/10.1016/j.susc.2020.121720· OSTI ID:1838426

Kao, Li Cheng ^[1]; Feng, Xuefei ^[2]; Ha, Yang ^[1]; Yang, Feipeng ^[2]; Liu, Yi-Sheng ^[1]; Hahn, Nathan T. ^[3]; MacDougall, James ^[1]; Chao, Weilun ^[1]; Yang, Wanli ^[1]; Zavadil, Kevin R. ^[3]; Guo, Jinghua ^[4]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Joint Center for Energy Storage Research, Lemont, IL (United States)
Joint Center for Energy Storage Research, Lemont, IL (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Joint Center for Energy Storage Research, Lemont, IL (United States); Univ. of California, Santa Cruz, CA (United States)

A method for performing X-ray absorption spectroscopy (XAS) in the soft X-ray region was developed to investigate the surface-sensitive electron signal of electrode/electrolyte interfaces in common multivalent based organic solvents under in situ/operando conditions. Our approach enables us to probe the molecular-scale structure of electrode interfaces by measuring total electron yield and is suitable for redox systems exhibiting low intrinsic electrochemical current. In-situ F K-edge XAS measurements in a 0.5 M Magnesium bis(trifluoromethanesulfonimide)/2-Methyltetrahydrofuran (Mg(TFSI)₂/2-MeTHF) electrolyte were carried out to determine the evolution of interfacial species during the electrochemical charging/discharging process. Time-dependent density-functional theory (TD-DFT) simulation indicate that the F K-edge evolution is the result of interfacial chemical environment change driven by electrochemical potential. In addition, we performed the “operando XAS” which runs the CV and collects spectra simultaneously. Furthermore, by using this method, the non-equilibrium state of condensed matter interfaces and interfacial dynamical transient process can be revealed.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1838426

Alternate ID(s):: OSTI ID: 1776224

Journal Information:: Surface Science, Journal Name: Surface Science Vol. 702; ISSN 0039-6028

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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In-situ/operando X-ray absorption spectroscopic investigation of the electrode/electrolyte interface on the molecular scale

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