Platinum‐Promoted Ga/Al<sub>2</sub>O<sub>3</sub> as Highly Active, Selective, and Stable Catalyst for the Dehydrogenation of Propane

Sättler, Jesper J. H. B.; Gonzalez-Jimenez, Ines D.; Luo, Lin; Stears, Brien A.; Malek, Andrzej; Barton, David G.; Kilos, Beata A.; Kaminsky, Mark; Verhoeven, Tiny; Koers, Eline J.; Baldus, Marc; Weckhuysen, Bert M.

doi:10.1002/anie.201404460

Cited by 236 publications

(226 citation statements)

References 38 publications

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“…In ar ecent study using Ga 2 O 3 /Al 2 O 3 -dopedP t and Ka st he catalyst, [21] the D/G ratio ranged from 0.73-1.00, with the coke amount varying from 0.23-0.55wt%.T he catalyst had as electivity that ranged from 65.8-96.9 %. Significant differencesb etweent he two families of catalysts can be observed from the data in the table.…”

Section: Coke Analysismentioning

confidence: 99%

“…The deconvolution procedure has been described in previouswork. [19,21] It should be noted that the absolutea mount of coke monotonically decreases as the gallium percentage decreases (IGA5-15-80 > IGA10-10-80 > IGA15- . The band at % 1200 cm À1 is assigned to ad isordered graphitic lattice, whereas the peak at % 1500 cm À1 is due to amorphous carbon.…”

Section: Coke Analysismentioning

confidence: 99%

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Propane Dehydrogenation over In₂O₃–Ga₂O₃–Al₂O₃ Mixed Oxides

et al. 2015

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A series of ternary mixed metal oxides containing Group III A elements (In, Ga, Al) is prepared by means of an alcoholic co‐precipitation method. Specifically, oxide catalysts with a molar composition of In/Ga/Al=5:15:80, 10:10:80, and 15:5:80 are reported. The chemical composition, redox properties, and catalyst structures are fully characterized, with the results suggesting that the indium, gallium, and aluminum moieties are well‐dispersed in the catalysts. The catalysts are evaluated for propane dehydrogenation (PDH) at 570 and 600 °C under 1 atm total pressure. The most effective catalyst with a composition of In/Ga/Al=5:15:80 provides 17 % conversion and approximately 86 % C3H6 selectivity with an initial activity of 4.6 mmol h−1 gcat−1 and 24.1 μmol h−1 m−2. The intrinsic activity on an active metal (i.e. indium and gallium) basis is approximately 3 times that of the In2O3–Ga2O3 family and approximately 3–9 times that of the In2O3–Al2O3 family. The catalyst deactivates with time on stream, and regeneration tests show that removal of surface coke and recovery of an In2O3 state helps to regain the initial activity, whereas reducing In2O3 domains into In0 does not allow for recovery of the performance. Raman analysis of the carbonaceous species deposited on the catalyst indicates catalysts with higher gallium content give more graphitic carbon, which correlates with higher C3H6 selectivity, whereas catalysts with more disordered coke are associated with lower selectivity. However, higher gallium content causes more coke formation, which leads to faster deactivation. This initial study of this family of mixed oxides suggests that an ideal In/Ga ratio may exist whereby catalyst properties may be optimized.

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Section: Coke Analysismentioning

confidence: 99%

Section: Coke Analysismentioning

confidence: 99%

Propane Dehydrogenation over In₂O₃–Ga₂O₃–Al₂O₃ Mixed Oxides

et al. 2015

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“…No dehydrogenation and decomposition reactivity was found on pure CeO 2 and Sn/CeO 2 .T his observation is consistent with an earlier report in which Pt catalysts with al ow loading (1000 ppm) presented poor activity for propane dehydrogenation. [12] To investigate the causes for the observed lack of selectivity of the single-atom Pt/CeO 2 material towards propylene,w ep erformed DFT calculations for Pt single atoms supported on CeO 2 (see Supporting Information). Pt adsorbs strongly at surface Ce 4+ vacancies;t he adsorption structures of pertinent species are displayed in Figures S2-S4 and the corresponding adsorption energies are listed in Table S1 (Supporting Information).…”

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confidence: 99%

Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria

et al. 2017

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Ceria (CeO 2 )s upports are unique in their ability to trap ionic platinum (Pt), providing exceptional stability for isolated single atoms of Pt. The reactivity and stability of single-atom Pt species was explored for the industrially important light alkane dehydrogenation reaction. The singleatom Pt/CeO 2 catalysts are stable during propane dehydrogenation, but are not selective for propylene.D FT calculations show strong adsorption of the olefin produced, leading to further unwanted reactions.Incontrast, when tin (Sn) is added to CeO 2 ,t he single-atom Pt catalyst undergoes an activation phase where it transforms into Pt-Sn clusters under reaction conditions.F ormation of small Pt-Sn clusters allows the catalyst to achieve high selectivity towards propylene because of facile desorption of the product. The CeO 2 -supported Pt-Sn clusters are very stable,e ven during extended reaction at 680 8 8C. Coke formation is almost completely suppressed by adding water vapor to the feed. Furthermore,u pon oxidation the Pt-Sn clusters readily revert to the atomically dispersed species on CeO 2 ,m aking Pt-Sn/CeO 2 af ully regenerable catalyst.

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“…According to the literature, activation of the first C−H bond in CH 4 was the rate‐determining step in methane combustion. Recently, Weckhuysen′s group have pointed out that modification of the Pt surface by gallium oxide primarily led to an increase in catalytic performance for propane dehydrogenation, and the authors explained that the coordinately unsaturated Ga 3+ species were responsible for the activation of the C−H bond and the dissociative adsorption of propane resulted in formation of a surface GaH/GaOH species. In the present work, a clear synergistic effect was observed between the Pd and GaO x components.…”

Section: Discussionmentioning

confidence: 99%

Highly Active and Stable Pd−GaO_x/Al₂O₃ Catalysts Derived from Intermetallic Pd₅Ga₃ Nanocrystals for Methane Combustion

et al. 2018

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Catalytic combustion of methane is widely used in industrial and transportation activities. The commonly used Pd‐based catalysts, however, are easily deactivated under hydrothermal conditions. In this work, we adopted a novel strategy to prepare a GaOx‐doped Pd/Al2O3 catalyst via the oxidative transformation of intermetallic Pd5Ga3 nanocrystals supported on γ‐Al2O3. We observed a synergistic effect between palladium and gallium oxide via formation of a bi‐functional active Pd−O−Ga phase, resulting in a highly active and exceptionally stable catalyst that could markedly suppress the sintering of noble metals under harsh conditions (hydrothermal treatment at 750 °C). Moreover, the presence of a large amount of surface oxygen vacancies and the surface Pd−O−Ga phase could promote methane combustion over the catalysts. It is believed that such a novel dual‐metal catalyst is promising in practical applications for methane combustion.

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Platinum‐Promoted Ga/Al₂O₃ as Highly Active, Selective, and Stable Catalyst for the Dehydrogenation of Propane

Cited by 236 publications

References 38 publications

Propane Dehydrogenation over In₂O₃–Ga₂O₃–Al₂O₃ Mixed Oxides

Propane Dehydrogenation over In₂O₃–Ga₂O₃–Al₂O₃ Mixed Oxides

Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria

Highly Active and Stable Pd−GaO_x/Al₂O₃ Catalysts Derived from Intermetallic Pd₅Ga₃ Nanocrystals for Methane Combustion

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Platinum‐Promoted Ga/Al2O3 as Highly Active, Selective, and Stable Catalyst for the Dehydrogenation of Propane

Cited by 236 publications

References 38 publications

Propane Dehydrogenation over In2O3–Ga2O3–Al2O3 Mixed Oxides

Propane Dehydrogenation over In2O3–Ga2O3–Al2O3 Mixed Oxides

Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria

Highly Active and Stable Pd−GaOx/Al2O3 Catalysts Derived from Intermetallic Pd5Ga3 Nanocrystals for Methane Combustion

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Platinum‐Promoted Ga/Al₂O₃ as Highly Active, Selective, and Stable Catalyst for the Dehydrogenation of Propane

Propane Dehydrogenation over In₂O₃–Ga₂O₃–Al₂O₃ Mixed Oxides

Propane Dehydrogenation over In₂O₃–Ga₂O₃–Al₂O₃ Mixed Oxides

Highly Active and Stable Pd−GaO_x/Al₂O₃ Catalysts Derived from Intermetallic Pd₅Ga₃ Nanocrystals for Methane Combustion