Dataset Information

Solvent Polarity-Induced Pore Selectivity in H-ZSM-5 Catalysis.

ABSTRACT: Molecular-sized micropores of ZSM-5 zeolite catalysts provide spatial restrictions around catalytic sites that allow for shape-selective catalysis. However, the fact that ZSM-5 has two main pore systems with different geometries is relatively unexploited as a potential source of additional shape selectivity. Here, we use confocal laser-scanning microscopy to show that by changing the polarity of the solvent, the acid-catalyzed furfuryl alcohol oligomerization can be directed to selectively occur within either of two locations in the microporous network. This finding is confirmed for H-ZSM-5 particles with different Si/Al ratios and indicates a general trend for shape-selective catalytic reactions.

SUBMITTER: Kubarev AV

PROVIDER: S-EPMC5504957 | biostudies-literature | 2017 Jul

REPOSITORIES: biostudies-literature

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Publications

Solvent Polarity-Induced Pore Selectivity in H-ZSM-5 Catalysis.

Kubarev Alexey V AV Breynaert Eric E Van Loon Jordi J Layek Arunasish A Fleury Guillaume G Radhakrishnan Sambhu S Martens Johan J Roeffaers Maarten B J MBJ

ACS catalysis 20170522 7

Molecular-sized micropores of ZSM-5 zeolite catalysts provide spatial restrictions around catalytic sites that allow for shape-selective catalysis. However, the fact that ZSM-5 has two main pore systems with different geometries is relatively unexploited as a potential source of additional shape selectivity. Here, we use confocal laser-scanning microscopy to show that by changing the polarity of the solvent, the acid-catalyzed furfuryl alcohol oligomerization can be directed to selectively occur ...[more]

PMID: 28713643

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Project description:In this work we demonstrate the selective catalytic conversion of prenol, which is an allylic alcohol that can be prepared from renewable resources to isoprene. The catalyst is an inexpensive molybdenum complex (Molyvan L) designed and used as an additive for lubricants. Isoprene is generated under relatively mild reaction parameters at 130-150°C, for 2 h, under vapor pressure conditions that do not exceed 50 psi. Two cases were studied: one in which Molyvan L was dissolved in a base oil at 1% concentration (weight/weight) and then mixed with a solvent and prenol and the other in which neat Molyvan L was introduced in the reaction and the base oil was replaced with the solvent and prenol. We investigated the selectivity of the reaction using the following solvents in both cases: dodecane, dodecanol, isododecane, octane, blendstock for oxygenate blending (BOB3), a fuel surrogate, a polyalphaolefin (PAO4), and methoxy polyethylene glycol (methoxy PEG350). Although conversion of prenol was above 94% in all experiments, isoprene was formed with various degrees of efficiency alongside a prenol isomeric alcohol, diprenyl ether and mixed ether via intramolecular and intermolecular dehydration reactions. Dodecane appeared to have the highest level of selectivity initially in base oil so we studied the effect of various dodecane-like solvents on isoprene yield and product profile. Surprisingly, octane (similar to dodecane) and isododecane (branched alkane) generated insignificant amounts of byproducts, essentially providing the highly desired isoprene with a very high selectivity. Branching of the solvent does not appear to have an effect on selectivity. Another advantage of this catalyst is the low loadings required to effect the transformation; that is, 0.25% (weight/volume) in the cases using neat Molyvan L and 0.5% (weight/volume) in the cases using Molyvan L dissolved in the base oil. Provided that prenol can be produced in large scale from bioresources, this work would enable the sustainable production of isoprene, in good yield, and with very high selectivity.

Dataset Information

Solvent Polarity-Induced Pore Selectivity in H-ZSM-5 Catalysis.

Publications

Solvent Polarity-Induced Pore Selectivity in H-ZSM-5 Catalysis.

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