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

Bauer T, Maisel S, Blaumeiser D, Vecchietti J, Taccardi N, Wasserscheid P, Bonivardi A, Görling A, Libuda J (2019)

Publication Type: Journal article

Publication year: 2019

Journal

ACS Catalysis American Chemical Society

Book Volume: 9

Pages Range: 2842-2853

Journal Issue: 4

DOI: 10.1021/acscatal.8b04578

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.

Authors with CRIS profile

Tanja Retzer Lehrstuhl für Physikalische Chemie II Sven Maisel Lehrstuhl für Theoretische Chemie Dominik Blaumeiser Lehrstuhl für Physikalische Chemie II Nicola Taccardi Lehrstuhl für Chemische Reaktionstechnik Peter Wasserscheid Lehrstuhl für Chemische Reaktionstechnik Andreas Görling Lehrstuhl für Theoretische Chemie Jörg Libuda Professur für Physikalische Chemie

Involved external institutions

National University of the Littoral / Universidad Nacional del Litoral (UNL) AR Argentina (AR)

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.

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