Catalytic properties of Pt-based intermetallic compounds in dehydrogenation of cyclohexane and n-butane

Furukawa, Shinya; Tamura, Asako; Ozawa, K.; Komatsu, Takayuki

doi:10.1016/j.apcata.2013.10.012

Cited by 49 publications

(44 citation statements)

References 33 publications

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“…14 Pt 3 Sn/SiO 2 exhibited not only higher selectivity but also greater catalytic activity than Pt/ SiO 2 in n-butane dehydrogenation to butenes. 15 Although this Pt-based catalyst showed high catalytic performance in dehydrogenation of n-butane, the high oxidizing ability of Pt may result in a larger amount of combustion to CO x in the oxidative dehydrogenation condition. Therefore, we focused on Pd-based intermetallic compounds as candidates of effective catalysts for oxidative dehydrogenation of 1-butene.…”

Section: ■ Introductionmentioning

confidence: 99%

Bifunctional Catalytic System Effective for Oxidative Dehydrogenation of 1-Butene and n-Butane Using Pd-Based Intermetallic Compounds

2014

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The catalytic performance of Pd-based intermetallic compounds supported on silica (Pd m M n /SiO 2 : M = Bi, Fe, Ge, In, Sn, Zn) was investigated in oxidative dehydrogenation of 1-butene and nbutane. A remarkable increase in selectivity (and also yield) of dehydrogenation products (1,3-butadiene and/or 1-butene) was obtained when PdIn, PdBi, or Pd 3 Fe replaced monometallic Pd. Temperature-programmed reduction and X-ray diffraction (XRD) studies on the catalysts with various treatments (i.e., the fresh, spent, and calcined) suggested that redox of the second metal was involved in the catalysis. XRD, X-ray photoelectron spectra, and transmission electron microscopy−energy dispersive X-ray spectroscopy analyses using the spent PdIn/SiO 2 catalyst revealed the formation of a core−shell structure consisting of a PdIn 1−δ core and Pd−In 2 O 3 composite shell formed by oxidative decomposition of PdIn during the reaction. A mechanistic study suggested that the presence of In atoms, adjacent to Pd atoms, effectively inhibits the undesired combustion by capturing O 2 as lattice oxygen. The incorporated lattice oxygen reacts with hydrogen atoms derived from the hydrocarbon by C−H activation over Pd sites, resulting in the formation of water and oxygen vacancy and/or the parent intermetallic phase. We thus reveal that a combination of C−H activation by Pd and the redox of the second metal provides a unique and effective dehydrogenation system.

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Section: ■ Introductionmentioning

confidence: 99%

Bifunctional Catalytic System Effective for Oxidative Dehydrogenation of 1-Butene and n-Butane Using Pd-Based Intermetallic Compounds

2014

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“…1,2,3,4 For example, compared to simple, single element metals, binary 10-14 intermetallics show enhanced catalytic activity, selectivity, and durability. 5,6,7 Among these, Pt-Sn nanocatalysts such as Pt3Sn and PtSn have been studied for a variety of reactions including alkane dehydrogenation, 8,9,10,11,12,13,14,15,16,17,18,19,20 electro-oxidation of CO, formic acid, and methanol fuel cells, 21,22,23,24,25,26 methane conversion to ethylene, benzene, and napththalene, 27 dehydroisomerization of butane to isobutene, 28 and highly selective hydrogenation of nitrobenzene to aniline, 29 3-nitrostyrene to 3-aminostyrene, 30 and of furfural to furfuryl alcohol. 31 Less studied are Pd-Sn and Ni-Sn binaries.…”

Section: Introductionmentioning

confidence: 99%

Intermetallic Nanocatalysts from Heterobimetallic Group 10–14 Pyridine-2-thiolate Precursors

et al. 2020

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Intermetallic compounds are atomically ordered inorganic materials containing two or more transition metals and main-group elements in unique crystal structures. Intermetallics based on group 10 and group 14 metals have shown enhanced activity, selectivity, and durability in comparison to simple metals and alloys in many catalytic reactions. While high-temperature solid-state methods to prepare intermetallic compounds exist, softer synthetic methods can provide key advantages, such as enabling the preparation of metastable phases or of smaller particles with increased surface areas for catalysis. Here, we study a generalized family of heterobimetallic precursors to binary intermetallics, each containing a group 10 metal and a group 14 tetrel bonded together and supported by pincer-like pyridine-2-thiolate ligands. Upon thermal decomposition, these heterobimetallic complexes form 10-14 binary intermetallic nanocrystals. Experiments and density functional theory (DFT) computations help in better understanding the reactivity of these precursors toward the synthesis of specific intermetallic binary phases. Using Pd2Sn as an example, we demonstrate that nanoparticles made in this way can act as uniquely selective catalysts for the reduction of nitroarenes to azoxyarenes, which highlights the utility of the intermetallics made by our method. Employing heterobimetallic pincer complexes as precursors toward binary nanocrystals and other metal-rich intermetallics provides opportunities to explore the fundamental chemistry and applications of these materials.

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“…Furukawa, Tamura, Ozawa, and Komatsu (2014) prepared Pt-based intermetallic catalysts, which were supported on silica (PtmMn/SiO 2 : M ¼ Co, Ge, Sn, Tl, and Zn). They studied the effect of the addition of a small amount of noble metal (1 wt% Pt, Pd, Rh) and concluded that 10 wt% Ag/1 wt% Pt and 10 wt% Ag/1 wt% Rh supported on activated carbon cloth are potential catalysts.…”

Section: An Overview On Cyclohexane Dehydrogenationmentioning

confidence: 99%

Butene oligomerization, phenol synthesis from benzene, butane partial oxidation, and other reactions carried out in membrane reactors

Rahimpour

2015

Membrane Reactors for Energy Applications and Basic Chemical Production

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Catalytic properties of Pt-based intermetallic compounds in dehydrogenation of cyclohexane and n-butane

Cited by 49 publications

References 33 publications

Bifunctional Catalytic System Effective for Oxidative Dehydrogenation of 1-Butene and n-Butane Using Pd-Based Intermetallic Compounds

Bifunctional Catalytic System Effective for Oxidative Dehydrogenation of 1-Butene and n-Butane Using Pd-Based Intermetallic Compounds

Intermetallic Nanocatalysts from Heterobimetallic Group 10–14 Pyridine-2-thiolate Precursors

Butene oligomerization, phenol synthesis from benzene, butane partial oxidation, and other reactions carried out in membrane reactors

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