Performance of Non-stoichiometric Perovskite Catalyst (A x CrO3−δ, A: La, Pr, Nd) for Dehydrogenation of Propane Under Steam Condition

Watanabe, Ryo; Tsujioka, Masahiro; Fukuhara, Choji

doi:10.1007/s10562-016-1876-5

Cited by 12 publications

(5 citation statements)

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“…Pure or partially substituted (A,A′,A′′)(B,B′,B′′)(O,X) 3 perovskites have been studied in various catalytic applications, , including oxygen evolution in alkaline solution, photocatalytic applications, CO oxidation, DeNO x reactions, and total combustion of alkanes and volatile organic compounds, ,− with the aim to replace noble metals as catalytically active components. Perovskites were implemented in oxygen-permeable membranes used in membrane reactors for selective oxidation of methane and other short-chain alkanes to higher hydrocarbons and olefins. − Olefins were synthesized at high temperatures over perovskite-supported platinum catalysts in the catalytic partial oxidation of ethane applying short contact times, in catalytic dehydrogenation of propane in the presence of steam, , and in oxidative dehydrogenation of propane applying chemical looping technologies or pulse experiments to control the activation of molecular oxygen on the surface of the perovskite catalyst. , …”

Section: Introductionmentioning

confidence: 99%

“…Perovskites were implemented in oxygen-permeable membranes used in membrane reactors for selective oxidation of methane and other short-chain alkanes to higher hydrocarbons and olefins. 15−17 Olefins were synthesized at high temperatures over perovskite-supported platinum catalysts in the catalytic partial oxidation of ethane applying short contact times, 18 in catalytic dehydrogenation of propane in the presence of steam, 19,20 dehydrogenation of propane applying chemical looping technologies or pulse experiments to control the activation of molecular oxygen on the surface of the perovskite catalyst. 21,22 The most productive catalysts so far in the activation of short-chain hydrocarbons under oxidative conditions are based on vanadium oxides.…”

Section: ■ Introductionmentioning

confidence: 99%

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Surface Conditions That Constrain Alkane Oxidation on Perovskites

et al. 2020

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The crystal structure of perovskites can incorporate a wide variety of cations, which makes this class of materials so interesting for studies of links between solid-state chemistry and catalysis. Perovskites are known as typical total combustion catalysts in hydrocarbon oxidation reactions. The fundamental question that we investigate here is whether surface modifications of perovskites can lead to the formation of valuable reaction products in alkane oxidation. We studied the effect of segregated two-dimensional surface nanostructures on selectivity to propene in the oxidative dehydrogenation of propane. Manganese-based perovskites AMnO 3 (A = La, Sm) were prepared by combustion and hydrothermal synthesis. Bulk and surface structures were investigated by X-ray diffraction, temperature-programmed reduction, aberration-corrected scanning transmission electron microscopy (STEM), multiwavelength Raman, and ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) in combination with near-edge X-ray absorption fine structure (NEXAFS) spectroscopy. Surface oxygen species responsible for C−H activation were distinguished by AP-XPS on the basis of a rigorous in situ analysis of the O 1s spectra recorded under a broad range of reaction conditions. Signals at 529.2, 530.1, 530.9, 531.2, and 531.8 eV were attributed to lattice O, defect-affected O, surface O, oxygen in carbonates, and hydroxyl groups, respectively. Operando AP-XPS revealed critical surface features, which occur under catalyst operation. The catalyst performance depends on the synthesis technique and the reaction conditions. In presence of a two-dimensional MnO x surface phase, addition of steam to the feed resulted in an increase in selectivity to the partial oxidation product propene to practically relevant values. The selectivity increase is related to the presence of Mn in a low oxidation state (2+/3+), an increased concentration of hydroxyl groups, and a higher abundance of adsorbed activated oxygen species on the catalyst surface. The surface analysis of a working catalyst highlights the importance of the termination layer of polycrystalline perovskites as a genuine property implemented by catalyst preparation. Such a termination layer controls the chemical properties and reactivity of perovskites. The information provides input for the development of realistic models that can be used by theory to predict functional properties.

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Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Surface Conditions That Constrain Alkane Oxidation on Perovskites

et al. 2020

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“…According to Asakura and Iwasawa 25) , the MgFe2O4 spinel phase is formed in the Fe/MgO catalyst due to the dispersion of Fe 3＋ on the MgO matrix during the impregnation process. /γ-Al 2 O 3 at 600 ºC 13) , Nd 0.95 CrO 3-δ at 625 ºC 22) , LaCo 0.2 Mn 0.8 O 3 at 650 ºC 23) First, Fe 3＋ is anchored to the OH group on the MgO surface, and MgFe2O4 is generated after calcination. For all the investigated catalysts, after PDH with co-feeding of H2S, the initially present α-Fe2O3 structure was converted to the pyrrhotite (Fe1-xS) structure due to the sulfidation of α-Fe2O3.…”

Section: Surface Area and Bulk Structure Of Various Fe-based Catalystsmentioning

confidence: 99%

Effect of Support Species on Performance of Transition Metal-based Catalysts for Propane Dehydrogenation with Co-feeding of H<sub>2</sub>S

Watanabe

Hirata

Yoda

et al. 2020

J. Jpn. Petrol. Inst.

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This study investigated the effect of catalyst supports (SiO2, γ-Al2O3, ZrO2, CeO2, MgO) on the performance of transition metal (Fe, Co, Ni) catalysts for propane dehydrogenation (PDH) with co-feeding of hydrogen sulfide (H2S). Evaluation of the catalyst activity indicated that inert SiO2 is a suitable support for the PDH catalysts. The SiO2-supported Fe catalysts showed the highest activity and selectivity among the investigated catalysts. In order to clarify the effect of the support species on the structure and electronic state of the catalyst components, X-ray diffraction (XRD), X-ray absorption fine structure (XAFS), and X-ray photoelectron spectroscopy (XPS) were used to characterize the various Fe-loaded catalysts. From Fe K-edge X-ray absorption near edge structure (XANES) analysis, it is deduced that the catalysts in which Fe was in a higher oxidation state showed better performance for PDH with co-feeding of H2S. When SiO2 and Al2O3 were used as the supports, divalent and trivalent Fe cations were detected by XPS analysis. Such high-valence Fe species can accept an electron from an intermediate species, thereby enhancing the dehydrogenation performance.

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“…Few reports have described the dehydrogenation of hydrocarbon under co-feeding of steam on the perovskite-type oxides. [17][18][19][20] To develop a catalyst with high selectivity and stability for EDH with steam, we specically examined Cr based perovskite catalyst. This study proposes a novel catalyst of YCrO 3 perovskite, which exhibits very high activity, selectivity, and stability in the steam-based dehydrogenation of ethane.…”

Section: Introductionmentioning

confidence: 99%