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

Tanja Bauer | Zendy; Sven Maisel | Zendy; Dominik Blaumeiser | Zendy; Julia Vecchietti | Zendy; Nicola Taccardi | Zendy; Peter Wasserscheid | Zendy; Adrián L. Bonivardi | Zendy; Andreas Görling | Zendy; Jörg Libuda | Zendy

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

Author(s) -

Tanja Bauer,

Sven Maisel,

Dominik Blaumeiser,

Julia Vecchietti,

Nicola Taccardi,

Peter Wasserscheid,

Adrián L. Bonivardi,

Andreas Görling,

Jörg Libuda

Publication year - 2019

Publication title -

acs catalysis

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 4.898

H-Index - 198

ISSN - 2155-5435

DOI - 10.1021/acscatal.8b04578

Subject(s) - dehydrogenation , propane , catalysis , adsorption , chemistry , diffuse reflectance infrared fourier transform , matrix isolation , diffuse reflection , inorganic chemistry , metal , infrared spectroscopy , platinum , heterogeneous catalysis , photochemistry , analytical chemistry (journal) , organic chemistry , photocatalysis , physics , optics

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/Al 2 O 3 , Pt/Al 2 O 3 , and Ga 37 Pt/Al 2 O 3 catalysts, to investigate in detail the nature of the active Pt species. Comparison of CO adsorption on Pt/Al 2 O 3 and Ga 37 Pt/Al 2 O 3 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/Al 2 O 3 , Pt/Al 2 O 3 , and Ga 37 Pt/Al 2 O 3 systems under operando conditions during propane dehydrogenation in CO/propane and in Ar/propane. We find that the Pt/Al 2 O 3 sample is rapidly poisoned by CO adsorption and coke, whereas propane dehydrogenation over Ga 37 Pt/Al 2 O 3 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.

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