Productive sugar isomerization with highly active Sn in dealuminated β zeolites

Dijkmans, Jan; Gabriëls, Dries; Dusselier, Michiel; Clippel, Filip de; Vanelderen, Pieter; Houthoofd, Kristof; Malfliet, Annelies; Pontikes, Yiannis; Sels, Bert F.

doi:10.1039/c3gc41239c

Cited by 245 publications

(263 citation statements)

References 54 publications

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“…As shown in Figure 1(c), weak peaks at 33.6°, 36.0°, and 41.4°, assignable to β-Si 3 N 4 derived from the milling pot and balls, are slightly apparent after the grinding for 24 h. The UV-vis spectrum of the SnO 2 -SiO 2 precursor before grinding exhibited a broad absorption band at approximately 260 nm (Figure 2(a)). The absorption behavior is consistent with a crystalline SnO 2 powder with octahedral Sn 4+ spaces [22,27]. On the other hand, a broad and strong absorption at approximately 200 nm is observed by the grinding for 12 h, and the absorption band at approximately 260 nm before grinding is shifted to a lower wavelength (Figure 2(b)).…”

Section: Resultssupporting

confidence: 76%

“…Therefore, the development of a novel procedure for obtaining MFI-type silicates with a high Sn 4+ content in the framework remains an important scientific goal [19–21]. As a new method, dealumination of silicates followed by the substitution of Sn 4+ atoms is a unique and practical technique for obtaining tailor-made-type zeolites [22]. However, the method has a potential problem from the production of inactive Sn species, such as SnO 2 on the extra-framework by the increase in the initial feeding amount of Sn 4+ ions.…”

Section: Introductionmentioning

confidence: 99%

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Mechanochemically assisted hydrothermal synthesis of Sn-substituted MFI-type silicates

Kanie

Sakaguchi

Muto

et al. 2018

Science and Technology of Advanced Materials

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Substitution of Al atoms in a zeolite framework by catalytic metal atoms has attracted considerable attention because the catalytic behavior can be tuned by the substituted atoms. In the present study, Sn-substituted MFI-type silicates were synthesized using a hydrothermal reaction of an amorphous Si-O-Sn precursor prepared by mechanochemical grinding of SiO2 and Sn(OH)4. The mechanochemical treatment was found to be a key technique for obtaining the amorphous Si-O-Sn precursor, where tetrahedral Sn4+ species were incorporated into the amorphous matrix. The Sn content in the framework of the MFI-type silicates was successfully controlled by the initial HCl/Si molar ratio of the hydrothermal procedures. Optical reflectance measurements revealed that the Sn4+ ions were dispersedly incorporated into the silicate framework while preserving the initial tetrahedrally coordinated species. Infrared results imply that the resulting Sn-substituted MFI-type silicate has Brønsted acid character. Precise control of the Brønsted and Lewis acid properties by Sn doping is a promising approach to the development of novel types of zeolite-based catalytic materials.

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Section: Resultssupporting

confidence: 76%

Section: Introductionmentioning

confidence: 99%

Mechanochemically assisted hydrothermal synthesis of Sn-substituted MFI-type silicates

Kanie

Sakaguchi

Muto

et al. 2018

Science and Technology of Advanced Materials

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“…[82] Nevertheless, Sn-b can be regenerated by calcination in air to restore its catalytic activity. [7,46,55] Filtration tests have demonstrated that the isomerization of glucose is truly heterogeneously catalyzed in the presence of Sn-b. [55] Leaching of Sn from hierarchical Sn-MFI during isomerizationh as been reported, though it can be suppressed by using ethanol or methanol as the solvent instead of water.…”

Section: Isomerization Over Lewis Acidsmentioning

confidence: 99%

“…Evenv ery concentrated solutions of glucose,u pt o4 5wt%,c an be successfully converted. [46] Sn-b has also been shown to be efficient in the isomerizationo fo ther carbohydrates such as xylose, [7,55,56,65] lyxose, [65a] ribose, [55, 65a] arabinose, [65a] mannose, [55, 65a] galactose, [55, 65a] and lactose. [56,66] The structure of the active centers and the mechanism of isomerization have recently been intensively studied by means of spectroscopic and computational tools,w ith af ocus mostly on glucosea sasubstrate.…”

Section: Isomerization Over Lewis Acidsmentioning

confidence: 99%

Catalytic Isomerization of Biomass‐Derived Aldoses: A Review

Delidovich

Palkovits

2016

ChemSusChem

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Invited for this month's cover are Irina Delidovich and Regina Palkovits from RWTH Aachen University. The mini‐installation of sugar cubes and granulated sugar with chemical equations of isomerization reactions written on it represents a renewable feedstock for producing a broad range of valuable products. Our Review summarizes recent advances on chemocatalytic isomerization. The Review itself is available at 10.1002/cssc.201501577.

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“…2,3 For this, a commercial β zeolite (CP814E, Zeolyst International, Si/Al = 25) was dealuminated by stirring it in a 7.2 M aqueous nitric acid solution at 353 K overnight. Afterwards, the powder was filtered, rinsed thoroughly with deionized water and dried overnight at 333 K. Prior to Sn grafting, the powder was activated overnight at 423 K to remove physisorbed water.…”

Section: Sn-β Deal Via Post-treatment Proceduresmentioning

confidence: 99%

Confinement Effects in Lewis Acid-Catalyzed Sugar Conversion: Steering Toward Functional Polyester Building Blocks

et al. 2015

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We report the use of solid Lewis acid catalysts for the conversion of tetrose sugars to four-carbon α-hydroxy acid esters (C4-AHA), which are useful as functional polyester building blocks. Sn-β was by far the most active and selective catalyst, yielding up to 80% methyl vinyl glycolate (MVG), methyl-4-methoxy-2-hydroxybutanoate (MMHB), and α-hydroxy-γ-butyrolactone (HBL) combined at 95% conversion. A very high turnover frequency (TOF) of 330 molC4‑AHA molSn h–1 was attained using Sn-β, a more than 6-fold increase compared with homogeneous SnCl4·5H2O. It is shown that, using different Sn-based catalysts with various pore sizes, the product distribution is strongly dependent on the size of the catalyst pores. Catalysts containing mainly mesopores, such as Sn-MCM-41 or Sn-SBA-15, prefer the production of the more bulky MMHB, whereas microporous catalysts such as Sn-β or Sn-MFI favor the production of MVG. This effect can be further enhanced by increasing the reaction temperature. At 363 K, only 20% MVG is attained using Sn-β, but at 433 K, this increases to 50%. Using a kinetic analysis, it was found that, in microporous catalysts, steric hindrance near the Sn active site in the catalyst pores plays a dominant role in favoring the reaction pathway toward MVG. Moreover, the selectivity toward both products is kinetically controlled.

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Productive sugar isomerization with highly active Sn in dealuminated β zeolites

Cited by 245 publications

References 54 publications

Mechanochemically assisted hydrothermal synthesis of Sn-substituted MFI-type silicates

Mechanochemically assisted hydrothermal synthesis of Sn-substituted MFI-type silicates

Catalytic Isomerization of Biomass‐Derived Aldoses: A Review

Confinement Effects in Lewis Acid-Catalyzed Sugar Conversion: Steering Toward Functional Polyester Building Blocks

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