Operando DRIFTS and DFT Study of Propane Dehydrogenation over Solid- and Liquid-Supported GaxPty Catalysts

Journal article


Publication Details

Author(s): Bauer T, Maisel S, Blaumeiser D, Vecchietti J, Taccardi N, Wasserscheid P, Bonivardi A, Görling A, Libuda J
Journal: ACS Catalysis
Publication year: 2019
Volume: 9
Journal issue: 4
Pages range: 2842-2853
ISSN: 2155-5435


Abstract

Supported catalytically active liquid metal solutions (SCALMS) represent a class of catalytic materials that have only recently been developed, but have already proven to be highly active, e.g., for dehydrogenation reactions. Previous studies attributed the catalytic activity to isolated noble metal atoms at the surface of a liquid and inert Ga matrix. In this study, we apply diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) with CO as a probe molecule to Ga/Al2O3, Pt/Al2O3, and Ga37Pt/Al2O3 catalysts, to investigate in detail the nature of the active Pt species. Comparison of CO adsorption on Pt/Al2O3 and Ga37Pt/Al2O3 shows that isolated Pt atoms are, indeed, present at the surface of the liquid SCALMS. Combining DRIFTS with online gas chromatography (GC), we investigated the Ga/Al2O3, Pt/Al2O3, and Ga37Pt/Al2O3 systems under operando conditions during propane dehydrogenation in CO/propane and in Ar/propane. We find that the Pt/Al2O3 sample is rapidly poisoned by CO adsorption and coke, whereas propane dehydrogenation over Ga37Pt/Al2O3 SCALMS leads to higher conversion with no indication of poisoning effects. We show under operando conditions that isolated Pt atoms are present at the surface of SCALMS during the dehydrogenation reaction. IR spectra and density-functional theory (DFT) suggest that both the Ga matrix and the presence of coadsorbates alter the electronic properties of the surface Pt species.


FAU Authors / FAU Editors

Bauer, Tanja
Lehrstuhl für Physikalische Chemie II
Blaumeiser, Dominik
Lehrstuhl für Physikalische Chemie II
Görling, Andreas Prof. Dr.
Lehrstuhl für Theoretische Chemie
Libuda, Jörg Prof. Dr.
Professur für Physikalische Chemie
Maisel, Sven
Lehrstuhl für Theoretische Chemie
Taccardi, Nicola Dr.
Lehrstuhl für Chemische Reaktionstechnik
Wasserscheid, Peter Prof. Dr.
Lehrstuhl für Chemische Reaktionstechnik


External institutions
National University of the Littoral


How to cite

APA:
Bauer, T., Maisel, S., Blaumeiser, D., Vecchietti, J., Taccardi, N., Wasserscheid, P.,... Libuda, J. (2019). Operando DRIFTS and DFT Study of Propane Dehydrogenation over Solid- and Liquid-Supported GaxPty Catalysts. ACS Catalysis, 9(4), 2842-2853. https://dx.doi.org/10.1021/acscatal.8b04578

MLA:
Bauer, Tanja, et al. "Operando DRIFTS and DFT Study of Propane Dehydrogenation over Solid- and Liquid-Supported GaxPty Catalysts." ACS Catalysis 9.4 (2019): 2842-2853.

BibTeX: 

Last updated on 2019-24-04 at 08:32