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“One-pot synthesis of Pt catalysts based on layered double hydroxides: an application in propane dehydrogenation”. Filez M, Redekop EA, Poelman H, Galvita VV, Meledina M, Turner S, Van Tendeloo G, Detavernier C, Marin GB, Catalysis science &, technology 6, 1863 (2016). http://doi.org/10.1039/C5CY01274K
Abstract: Simple methods for producing noble metal catalysts with well-defined active sites and improved performance are highly desired in the chemical industry. However, the development of such methods still presents a formidable synthetic challenge. Here, we demonstrate a one-pot synthesis route for the controlled production of bimetallic Pt–In catalysts based on the single-step formation of Mg,Al,Pt,In-containing layered double hydroxides (LDHs). Besides their simple synthesis, these Pt–In catalysts exhibit superior propane dehydrogenation activity compared to their multi-step synthesized analogs. The presented material serves as a showcase for the one-pot synthesis of a broader class of LDH-derived mono- and multimetallic Pt catalysts. The compositional flexibility provided by LDH materials can pave the way towards highperforming Pt-based catalysts with tunable physicochemical properties.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.773
Times cited: 12
DOI: 10.1039/C5CY01274K
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“Towards biolubricant compatible vegetable oils by pore mouth hydrogenation with shape-selective Pt/ZSM-5 catalysts”. Van Aelst J, Philippaerts A, Bartholomeeusen E, Fayad E, Thibault-Starzyk F, Lu J, Schryvers D, Ooms R, Verboekend D, Jacobs P, Sels B, Catalysis science &, technology 6, 2820 (2016). http://doi.org/10.1039/C6CY00498A
Abstract: Pt/ZSM-5 catalysts with various crystal sizes were prepared via competitive ion-exchange, followed by a slow activation procedure. Even when using very large ZSM-5 crystals, highly dispersed Pt nano-clusters were contained within the zeolite crystal's voids, as ascertained by 2D pressure-jump IR spectroscopy of adsorbed CO and focussed ion-beam transmission electron microscopy. The shape-selective properties of the Pt/ZSM-5 catalysts were evaluated in the partial hydrogenation of soybean oil. Unique hydrogenation selectivities were observed, as the fatty acids located at the central position of the triacylglycerol (TAG) molecules were preferentially hydrogenated. The resulting oil has therefore high levels of intermediately melting TAGs, which are compatible with biolubricants due to their improved oxidative stability and still appropriate low-temperature fluidity. The TAG distribution in the partially hydrogenated soybean oil samples was independent from the zeolite crystal size, while the hydrogenation activity linearly increases with the crystal's external surface area. This trend was confirmed with a Pt loaded mesoporous ZSM-5 zeolite, obtained via a mild alkaline treatment. These observations imply and confirm a genuine pore mouth catalysis mechanism, in which only one fatty acid chain of the TAG is able to enter the micropores of ZSM-5, where the double bonds are hydrogenated by the crystal encapsulated Pt-clusters.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.773
Times cited: 5
DOI: 10.1039/C6CY00498A
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“Observation of surface species in plasma-catalytic dry reforming of methane in a novel atmospheric pressure dielectric barrier discharge in situ IR cell”. Van Turnhout J, Aceto D, Travert A, Bazin P, Thibault-Starzyk F, Bogaerts A, Azzolina-Jury F, Catalysis Science &, Technology 12, 6676 (2022). http://doi.org/10.1039/D2CY00311B
Abstract: We developed a novel in situ (i.e. inside plasma and during operation) IR dielectric barrier discharge cell allowing investigation of plasma catalysis in transmission mode, atmospheric pressure, flow conditions (WHSV similar to 0-50 000 mL g(-1) h(-1)), at relevant discharge voltages (similar to 0-50 kV) and frequencies (similar to 0-5 kHz). We applied it to study the IR-active surface species formed on a SiO2 support and on a 3 wt% Ru/SiO2 catalyst, which can help to reveal the important surface reaction mechanisms during the plasma-catalytic dry reforming of methane (DRM). Moreover, we present a technique for the challenging task of estimating the temperature of a catalyst sample in a plasma-catalytic system in situ and during plasma operation. We found that during the reaction, water is immediately formed at the SiO2 surface, and physisorbed formic acid is formed with a delay. As Ru/SiO2 is subject to greater plasma-induced heating than SiO2 (with a surface temperature increase in the range of 70-120 degrees C, with peaks up to 150 degrees C), we observe lower amounts of physisorbed water on Ru/SiO2, and less physisorbed formic acid formation. Importantly, the formation of surface species on the catalyst sample in our plasma-catalytic setup, as well as the observed conversions and selectivities in plasma conditions, can not be explained by plasma-induced heating of the catalyst surface, but must be attributed to other plasma effects, such as the adsorption of plasma-generated radicals and molecules, or the occurrence of Eley-Rideal reactions.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 5
DOI: 10.1039/D2CY00311B
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“Factors driving the activity of commercial titanium dioxide powders towards gas phase photocatalytic oxidation of acetaldehyde”. Verbruggen SW, Masschaele K, Moortgat E, Korany TE, Hauchecorne B, Martens JA, Lenaerts S, Catalysis science &, technology 2, 2311 (2012). http://doi.org/10.1039/C2CY20123B
Abstract: The photocatalytic activity of two commercial titanium dioxide powders (Cristal Global, Millennium PC500 and Evonik, P25) is compared towards acetaldehyde degradation in the gas phase. In contrast to the extensive literature available, we found a higher activity for the PC500 than for the P25 coating. Here, we present a comprehensive characterization of the bulk and surface properties of both powders. Our comparison shows that the material properties that dominate the overall photocatalytic activity in gas phase differ from those required for the photodegradation of water-borne pollutants.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 5.773
Times cited: 33
DOI: 10.1039/C2CY20123B
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“Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene”. de la Croix T, Claes N, Eyley S, Thielemans W, Bals S, De Vos D, Catalysis Science &, Technology (2023). http://doi.org/10.1039/D3CY00370A
Abstract: The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.
Keywords: A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Impact Factor: 5
DOI: 10.1039/D3CY00370A
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