Gas Pulse-X-Ray Probe Ambient Pressure Photoelectron Spectroscopy with Submillisecond Time Resolution

Andrey Shavorskiy, Giulio D'Acunto, Virginia Boix De La Cruz, Mattia Scardamaglia, Suyun Zhu, Robert H. Temperton, Joachim Schnadt, Jan Knudsen

Research output: Contribution to journalArticlepeer-review

Abstract

A setup capable of conducting gas pulse-X-ray probe ambient pressure photoelectron spectroscopy with high time resolution is presented. The setup makes use of a fast valve that creates gas pulses with an internal pressure in the mbar range and a rising edge of few hundreds of microseconds. A gated detector based on a fast camera is synchronized with the valve operation to measure X-ray photoemission spectra with up to 20 μs time resolution. The setup is characterized in several experiments in which the N2 gas is pulsed either into vacuum or a constant flow of another gas. The observed width of the pulse rising edge is 80 μs, and the maximum internal pulse pressure is ∼1 mbar. The CO oxidation reaction over Pt (111) was used to demonstrate the capability of the setup to correlate the gas phase composition with that of the surface during transient supply of CO gas into an O2 stream. Thus, formation of both chemisorbed and oxide oxygen species was observed prior to CO gas perturbation. Also, the data indicated that both the Langmuir-Hinshelwood and Mars-van-Krevelen mechanisms play an important role in the oxidation of carbon monoxide under ambient conditions.

Original languageEnglish
Pages (from-to)47629–47641
Number of pages13
JournalACS Applied Materials and Interfaces
Volume13
Issue number40
DOIs
Publication statusPublished - 2021 Sep

Subject classification (UKÄ)

  • Atom and Molecular Physics and Optics
  • Accelerator Physics and Instrumentation

Keywords

  • APXPS
  • catalysis
  • CO oxidation
  • operando spectroscopy
  • time-resolved XPS

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