TY - JOUR
AU - Bauer, Tanja
AU - Maisel, Sven
AU - Blaumeiser, Dominik
AU - Vecchietti, Julia
AU - Taccardi, Nicola
AU - Wasserscheid, Peter
AU - Bonivardi, Adrian
AU - Görling, Andreas
AU - Libuda, Jörg
TI - Operando DRIFTS and DFT Study of Propane Dehydrogenation over Solid- and Liquid-Supported Ga x Pt y Catalysts
JO - ACS catalysis
VL - 9
IS - 4
SN - 2155-5435
CY - Washington, DC
PB - ACS
M1 - FZJ-2019-05453
SP - 2842 - 2853
PY - 2019
AB - 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.
LB - PUB:(DE-HGF)16
UR - <Go to ISI:>//WOS:000464075700012
DO - DOI:10.1021/acscatal.8b04578
UR - https://juser.fz-juelich.de/record/866294
ER -