Catalytic Dehydrogenation of Gaseous of Paraffins

Grosse, A. V.; Ipatieff, V. N.

doi:10.1021/ie50362a024

Cited by 23 publications

(14 citation statements)

References 5 publications

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“…[3] Subsequently, g-alumina found wide applications as as upport for organometallic molecular complexes,i solated ions,n anoparticles,e tc., [1] the latter becoming industrially relevant for automotive applications and petroleum refining. [4][5][6] Thep recise nature of the catalytically active surface sites of g-alumina remains obscure despite am ultitude of studies aimed at clarifying this uncertainty. [7][8][9][10][11][12] Theo rigin of this challenge lies in the complex crystalline structure of g-alumina which is still unresolved, and which evolves into the closely related deltaand theta-transitional aluminas with thermal treatments above 850 8 8C.…”

Section: Introductionmentioning

confidence: 99%

“…Since Vladimir Ipatieff's discovery in 1902 that γ‐alumina can be used as a robust large‐scale catalyst for ethanol dehydration to produce ethylene, [1, 2] this material has emerged as the oldest and most commercially important heterogeneous catalysts, featuring high surface area and excellent high‐temperature stability [3] . Subsequently, γ‐alumina found wide applications as a support for organometallic molecular complexes, isolated ions, nanoparticles, etc., [1] the latter becoming industrially relevant for automotive applications and petroleum refining [4–6] . The precise nature of the catalytically active surface sites of γ‐alumina remains obscure despite a multitude of studies aimed at clarifying this uncertainty [7–12] .…”

Section: Introductionmentioning

confidence: 99%

“…organometallic molecular complexes, isolated ions, nanoparticles, etc. [1], the latter becoming industrially relevant for automotive applications and petroleum refining [4][5][6]. The precise nature of the catalytically active surface sites of γ-alumina remains obscure despite a multitude of studies and ten decades of research aimed at revealing this uncertainty [7][8][9][10][11][12].…”

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confidence: 99%

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Precise Identification and Characterization of Catalytically Active Sites on the Surface of γ‐Alumina**

et al. 2021

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g-alumina is one of the oldest and most important commercial catalytic materials with high surface area and stability.These attributes enabled its use as the first commercial large-scale heterogeneous catalyst for ethanol dehydration. Despite progress in materials characterization the nature of the specific sites on the surface of g-alumina that are responsible for its unique catalytic properties has remained obscure and controversial. By using combined infrared spectroscopy, electron microscopya nd solid-state nuclear magnetic resonance measurements we identify the octahedral, amphoteric (O) 5 Al(VI)-OH sites on the (100) segments of massively restructured (110) facets on typical rhombus-platelet g-alumina as well as the (100) segments of irrational surfaces (invariably always present in all g-alumina samples) responsible for its unique catalytic activity.Such (O) 5 Al(VI)-OH sites are also present on the macroscopically defined (100) facets of g-alumina with elongated/rod-like geometry.T he mechanism by which these sites lose -OH groups upon thermal dehydroxylation resulting in coordinatively unsaturated penta-coordinate Al +3 O 5 sites is clarified. These coordinatively unsaturated penta-coordinate Al sites produce well-defined thermally stable Al-carbonyl complexes.O ur findings contribute to the understanding of the nature of coordinatively unsaturated Al sites on the surface of g-alumina and their role as catalytically active sites.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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confidence: 99%

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Precise Identification and Characterization of Catalytically Active Sites on the Surface of γ‐Alumina**

et al. 2021

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“…Chromium oxide-based catalysts have been one of the most actively investigated formulations for dehydrogenation since the first report of Frey and Huppke in 1933 . Dehydrogenation of butanes over a chromia/alumina catalyst was first developed in the 1940s at Leuna and independently at UOP by Ipatieff and co-workers. , These catalysts have been applied to several processes for dehydrogenation of light olefins. Several challenges in utilization of these catalysts were repeatedly highlighted, namely, a certain health risk, when the plant operators are exposed to Cr(VI)-containing catalysts, and sintering at high temperatures.…”

Section: Introductionmentioning

confidence: 99%

Recycling of Wastes from the Production of Alumina-Based Catalyst Carriers

Matveyeva

Пахомов

Murzin

2016

Ind. Eng. Chem. Res.

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Preparation of microspherical chromia−alumina KDM-type catalysts for alkane dehydrogenation is based on utilization of an amorphous nanostructured hydroxide−oxide Al 2 O 3 −x(OH) 2 •nH 2 O (where x = 0−0.28, n = 0.03−1.8) prepared via the centrifugal thermal activation (CTA) of gibbsite. The fine fraction of this carrier is considered as industrial waste, requiring efficient recycling options, which are explored in this work. A range of physicochemical methods was applied to analyze the main properties (phase composition, morphology, reactivity, etc.) of pilot and industrial batches of gibbsite CTA products. It has been clearly shown that the properties of CTA products are dependent on the nature of gibbsite used. The largest amount of the active amorphous phase of alumina is formed using gibbsite made from concentrated nepheline. Regularities of rehydration of the CTA-products fine fraction in acidic/ alkaline media and dissolution in sulfuric acid of the fine fraction of gibbsite and the industrial CTA product were explored to prepare aluminum sulfate, which is a water purification coagulant.

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“…Since then, it has remained one of the largest scale heterogeneous materials produced industrially. It features high surface area and attractive mechanical properties [2][3][4][5][6][7][8]. For this reason, γ-alumina found an application as a support for metals [1-8] (metal and metal oxide nanoparticles, single ions) for catalytic removal of nuisance pollutants in vehicles: the majority of alumina produced nowadays is used specifically for this very purpose.…”

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confidence: 99%

Phase and facet-engineering of transition alumina leads to (hydro)thermally stable alumina-supported metal catalysts

Khivantsev

Kwak

Jaegers

et al. 2021

Preprint

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Inherent thermal instability of gamma-alumina above 800-900 ⁰C leads to deactivation of noble metal-supported alumina catalysts used in automotive applications. This is typically solved by adding toxic (barium) and/or rare-earth (lanthanum, cerium) elements. We show that facet-dependent engineering of transition-alumina leads to (hydro)thermally stable supported metal catalysts in the absence of toxic and rare-earth additives. Since pure high-surface area theta-alumina can be prepared at 1,050-1,100 ⁰C directly from gamma-alumina (or boehmite), and because of its stable major (100) facet with very low surface energy of 597 mJ/m2, we succeeded in preparing ~0.07 wt% Rh and ~3 wt% Pd catalysts active in NO reduction and hydrocarbon oxidation that survive hydrothermal aging up to 1,100 ⁰C with little-to-no deactivation.

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Catalytic Dehydrogenation of Gaseous of Paraffins

Cited by 23 publications

References 5 publications

Precise Identification and Characterization of Catalytically Active Sites on the Surface of γ‐Alumina**

Precise Identification and Characterization of Catalytically Active Sites on the Surface of γ‐Alumina**

Recycling of Wastes from the Production of Alumina-Based Catalyst Carriers

Phase and facet-engineering of transition alumina leads to (hydro)thermally stable alumina-supported metal catalysts

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