EXAFS study of Pd/Ga2O3 model catalysts of selective liquid-phase hydrogenation of acetylene to ethylene

Смирнова, Н. С.; Shlyapin, D. A.; Mironenko, O. O.; Anoshkina, E. A.; Темерев, В. Л.; Шитова, Н. Б.; Kochubey, D. I.; Цырульников, П. Г.

doi:10.1016/j.molcata.2012.03.010

Cited by 14 publications

(10 citation statements)

References 23 publications

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“…The RMSI term refers to a chemical interaction on the metal–oxide surface under high reduction temperature, which leads to the alloy or IMCs formation. The widely used oxides for catalyst preparation comprise Ga 2 O 3 [ 6 , 10 , 18 ], GeO 2 [ 7 ], CeO 2 [ 19 ], ZnO [ 9 , 20 , 21 ], and In 2 O 3 [ 17 , 22 , 23 ]. The main problem using reactive metal-support interaction for the synthesis of supported IMC nanoparticles is that usually a mixture of IMCs with the supported metal (modifier) is formed.…”

Section: Introductionmentioning

confidence: 99%

Highly-Ordered PdIn Intermetallic Nanostructures Obtained from Heterobimetallic Acetate Complex: Formation and Catalytic Properties in Diphenylacetylene Hydrogenation

et al. 2018

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Formation of PdIn intermetallic nanoparticles supported on α-Al2O3 was investigated by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), and hydrogen temperature-programmed desorption (H2-TPD) methods. The metals were loaded as heterobimetallic Pd(μ-O2CMe)4In(O2CMe) complex to ensure intimate contact between Pd and In. Reduction in H2 at 200 °C resulted in Pd-rich PdIn alloy as evidenced by XRD and the disappearance of Pd hydride. A minor amount of Pd1In1 intermetallic phase appeared after reduction at 200 °C and its formation was accomplished at 400 °C. Neither monometallic Pd or in nor other intermetallic structures were found after reduction at 400–600 °C. Catalytic performance of Pd1In1/α-Al2O3 was studied in the selective liquid-phase diphenylacetylene (DPA) hydrogenation. It was found that the reaction rate of undesired alkene hydrogenation is strongly reduced on Pd1In1 nanoparticles enabling effective kinetic control of the hydrogenation, and the catalyst demonstrated excellent selectivity to alkene.

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Section: Introductionmentioning

confidence: 99%

Highly-Ordered PdIn Intermetallic Nanostructures Obtained from Heterobimetallic Acetate Complex: Formation and Catalytic Properties in Diphenylacetylene Hydrogenation

et al. 2018

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“…O 2 ‐TPD results confirm that the amount of lattice oxygen released from Pd−GaO x /Al 2 O 3 −HT was much lower as compared with the Pd−GaO x /Al 2 O 3 and Pd/Al 2 O 3 −HT samples, suggesting that the hydrothermal treatment could further benefit enhancement of the Pd−O−Ga bond strength. Taking these considerations together, we believe that during the heating process in air at higher temperatures, gallium oxide interacted with palladium oxide to yield a homogeneous solid solution or form a Pd−Ga−O compound, causing the lattice distortion of PdO x . In addition, hydrothermal treatment could also serve as an alternative strategy for preparing more stable supported catalysts.…”

Section: Discussionmentioning

confidence: 99%

“…Taking these considerations together, we believe that during the heating process in air at higher temperatures, gallium oxide interacted with palladium oxide to yield a homogeneous solid solution or form a PdÀ GaÀ O compound, causing the lattice distortion of PdO x . [52] In addition, hydrothermal treatment could also serve as an alternative strategy for preparing more stable supported catalysts. The presented data were consistent with the lowtemperature multistep pathway in which the intermetallic nanoparticles were oxidized into nanocrystalline multi-metal oxides (Figure 8), which would result in a very stable catalyst with high resistance to deactivation.…”

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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“…Briefly, the Pd/Ga 2 O 3 catalyst was selected as a model material, since it is regarded as an ideal catalyst for methanol steam reforming, selective hydrogenation of alkyne, and water‐gas shift reactions . The derived Pd 2 Ga structure can be prepared from the reduction of Ga 2 O 3 supported Pd, which exhibits superior catalytic performance in view of the unique electronic structure and ordered arrangement of Pd atoms.…”

Section: Figurementioning

confidence: 99%

Assessing the Effect of the Electron‐Beam Irradiation on Pd/Ga₂O₃ Catalyst under Ambient Pressure

et al. 2020

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Introducing atmosphere in transmission electron microscope enables to directly observe the structural features of catalyst under working conditions. It offers the possibility to study the microstructural evolution and correlate real structures with catalytic properties at nano‐ or atomic‐scale during catalysis. However, the damages to catalyst derived from the high energy electron‐beam irradiation cannot be ignored and may lead to ambiguous conclusions, as the interaction between reactive gas molecules and active structures is only desired. Herein, the α‐Ga2O3 supported Pd catalyst was selected as a model to evaluate the potential effect of electron‐beam on the surface and interface structures, which directly affect the catalytic performance, at varied atmospheres, elevated temperatures and increased electron dose rate in ambient pressure. The results indicate that the supported Pd nanoparticles could be encapsulated by GaOx layer when the imaging electron dose rate is higher than 100 e/Å2s under reduction and oxidizing atmosphere. Either increasing the electron dose rate or elevating the temperature exacerbates the irradiation damage to α‐Ga2O3 support. This work was expected to evaluate the effect of electron dose rate to supported catalysts under chemical environments, and provide guidance for the investigation of in‐situ transmission electron microscopy under ambient pressure.

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EXAFS study of Pd/Ga2O3 model catalysts of selective liquid-phase hydrogenation of acetylene to ethylene

Cited by 14 publications

References 23 publications

Highly-Ordered PdIn Intermetallic Nanostructures Obtained from Heterobimetallic Acetate Complex: Formation and Catalytic Properties in Diphenylacetylene Hydrogenation

Highly-Ordered PdIn Intermetallic Nanostructures Obtained from Heterobimetallic Acetate Complex: Formation and Catalytic Properties in Diphenylacetylene Hydrogenation

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

Assessing the Effect of the Electron‐Beam Irradiation on Pd/Ga₂O₃ Catalyst under Ambient Pressure

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EXAFS study of Pd/Ga2O3 model catalysts of selective liquid-phase hydrogenation of acetylene to ethylene

Cited by 14 publications

References 23 publications

Highly-Ordered PdIn Intermetallic Nanostructures Obtained from Heterobimetallic Acetate Complex: Formation and Catalytic Properties in Diphenylacetylene Hydrogenation

Highly-Ordered PdIn Intermetallic Nanostructures Obtained from Heterobimetallic Acetate Complex: Formation and Catalytic Properties in Diphenylacetylene Hydrogenation

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

Assessing the Effect of the Electron‐Beam Irradiation on Pd/Ga2O3 Catalyst under Ambient Pressure

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

Assessing the Effect of the Electron‐Beam Irradiation on Pd/Ga₂O₃ Catalyst under Ambient Pressure