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

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

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17 Citations (Scopus)

Abstract

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. By using this method, the non-equilibrium state of condensed matter interfaces and interfacial dynamical transient process can be revealed.

Original languageEnglish
Article number121720
JournalSurface Science
Volume702
DOIs
Publication statusPublished - 2020 Dec

All Science Journal Classification (ASJC) codes

  • Condensed Matter Physics
  • Surfaces and Interfaces
  • Surfaces, Coatings and Films
  • Materials Chemistry

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