Issue 27, 2023

Improving time-resolution and sensitivity of in situ X-ray photoelectron spectroscopy of a powder catalyst by modulated excitation

Abstract

Ambient pressure X-ray photoelectron spectroscopy (APXPS) is a powerful tool to characterize the surface structure of heterogeneous catalysts in situ. In order to improve the time resolution and the signal-to-noise (S/N) ratio of photoemission spectra, we collected consecutive APXP spectra during the periodic perturbation of a powder Pd/Al2O3 catalyst away from its equilibrium state according to the modulated excitation approach (ME). Averaging of the spectra along the alternate pulses of O2 and CO improved the S/N ratio demonstrating that the time resolution of the measurement can be limited solely to the acquisition time of one spectrum. Through phase sensitive analysis of the averaged time-resolved spectra, the formation/consumption dynamics of three oxidic species, two metal species, adsorbed CO on Pd0 as well as Pdn+ (n > 2) was followed along the gas switches. Pdn+ and 2-fold surface PdO species were recognised as most reactive to the gas switches. Our approach demonstrates that phase sensitive detection of time-resolved XPS data allows following the dynamics of reactive species at the solid–gas interface under different reaction environments with unprecedented precision.

Graphical abstract: Improving time-resolution and sensitivity of in situ X-ray photoelectron spectroscopy of a powder catalyst by modulated excitation

Associated articles

Supplementary files

Article information

Article type
Edge Article
Submitted
08 mar 2023
Accepted
29 may 2023
First published
30 may 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2023,14, 7482-7491

Improving time-resolution and sensitivity of in situ X-ray photoelectron spectroscopy of a powder catalyst by modulated excitation

M. Roger, L. Artiglia, A. Boucly, F. Buttignol, M. Agote-Arán, J. A. van Bokhoven, O. Kröcher and D. Ferri, Chem. Sci., 2023, 14, 7482 DOI: 10.1039/D3SC01274C

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