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Title: Reaction cell for in situ soft x-ray absorption spectroscopy and resonant inelastic x-ray scattering measurements of heterogeneous catalysis up to 1 atm and 250 °C

We present a novel in situ reaction cell for heterogeneous catalysis monitored in situ by x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS). The reaction can be carried out at a total pressure up to 1 atm, a regime that has not been accessible to comparable in situ techniques and thus closes the pressure gap to many industrial standard conditions. Two alternate catalyst geometries were tested: (A) a thin film evaporated directly onto an x-ray transparent membrane with a flowing reaction gas mixture behind it or (B) a powder placed behind both the membrane and a gap of flowing reaction gas mixture. To illustrate the working principle and feasibility of our reaction cell setup we have chosen ethylene epoxidation over a silver catalyst as a test case. The evolution of incorporated oxygen species was monitored by total electron/fluorescence yield O K-XAS as well as O K-RIXS, which is a powerful method to separate contributions from inequivalent sites. We find that our method can reliably detect transient species that exist during catalytic reaction conditions that are hardly accessible using other spectroscopic methods.
Authors:
 [1] ;  [2] ;  [2] ; ;  [3] ;  [4] ;  [1]
  1. Department of Physics and Astronomy, Division of Molecular and Condensed Matter Physics, Uppsala University, Box 516, S-751 20 Uppsala (Sweden)
  2. (Germany)
  3. Abteilung Anorganische Chemie, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin (Germany)
  4. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)
Publication Date:
OSTI Identifier:
22220320
Resource Type:
Journal Article
Resource Relation:
Journal Name: Review of Scientific Instruments; Journal Volume: 84; Journal Issue: 11; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; ABSORPTION SPECTROSCOPY; CATALYSTS; ETHYLENE; FLUORESCENCE; HETEROGENEOUS CATALYSIS; MEMBRANES; MIXTURES; SILVER; SOFT X RADIATION; THIN FILMS; X-RAY DIFFRACTION; X-RAY SPECTRA; X-RAY SPECTROSCOPY