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Self-assembled hybrid metal oxide base catalysts prepared by simply mixing with organic modifiers.

Nature communications (2015-10-06)
Masazumi Tamura, Ryota Kishi, Yoshinao Nakagawa, Keiichi Tomishige
ABSTRACT

Multidentate materials formed by simply mixing heterogeneous and homogeneous components are promising for construction of versatile active sites on the surface of heterogeneous compounds, however, to the best of our knowledge, there are no reports on such materials. Self-assembly of hetero-hybrid catalytic materials occurs when heterogeneous catalysts having adjacent Lewis acid-Lewis base sites are mixed with an organic modifier that contains at least two Lewis base functional groups. Here we demonstrate the strategy by combining cerium oxide and 2-cyanopyridine that self-assembles to form a charge-transfer complex in methanol that exhibits a 2,000-fold increase in reaction rate for hydromethoxylation of acrylonitrile with high selectivity compared with cerium oxide or 2-cyanopyridine alone. The catalytic system is applied to the transesterification and Knoevenagel condensation affording 14-fold and 11-fold higher activity, respectively, than cerium oxide alone. These results demonstrate the potential versatility of the catalytic system and the generality of the catalyst preparation strategy.

MATERIALS
Product Number
Brand
Product Description

Sigma-Aldrich
Methanol, anhydrous, 99.8%
Sigma-Aldrich
Acetone, ACS reagent, ≥99.5%
Sigma-Aldrich
Ethyl alcohol, Pure, 190 proof, ACS spectrophotometric grade, 95.0%
Sigma-Aldrich
Ethanol, purum, secunda spirit, denaturated with 2% 2-butanone and 0.5% 4-methyl-2-pentanone, S15, ~96% (based on denaturant-free substance)
Sigma-Aldrich
Pyridine, anhydrous, 99.8%
Sigma-Aldrich
1,4-Dioxane, anhydrous, 99.8%
Sigma-Aldrich
Methanol, ACS reagent, ≥99.8%
Sigma-Aldrich
Acetone, puriss. p.a., ACS reagent, reag. ISO, reag. Ph. Eur., ≥99.5% (GC)
Sigma-Aldrich
Benzaldehyde, ReagentPlus®, ≥99%
Sigma-Aldrich
Pyridine, ACS reagent, ≥99.0%
Sigma-Aldrich
Methanol, puriss. p.a., ACS reagent, reag. ISO, reag. Ph. Eur., ≥99.8% (GC)
Sigma-Aldrich
1,4-Dioxane, ACS reagent, ≥99.0%
Sigma-Aldrich
Dodecane, anhydrous, ≥99%
Sigma-Aldrich
Ethyl alcohol, Pure, 200 proof, meets USP testing specifications
Sigma-Aldrich
Benzaldehyde, purified by redistillation, ≥99.5%
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Acrylonitrile, ≥99%, contains 35-45 ppm monomethyl ether hydroquinone as inhibitor
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Methyl benzoate, 99%
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Acetone, Laboratory Reagent, ≥99.5%
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2,6-Lutidine, purified by redistillation, ≥99%
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Methanol, Laboratory Reagent, ≥99.6%
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Pyridine, ReagentPlus®, ≥99%
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1-Hexanol, anhydrous, ≥99%
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Furan, ≥99%
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Dodecane, ReagentPlus®, ≥99%
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Ethyl cyanoacetate, ≥98%
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2-Picolinic acid, ReagentPlus®, 99%
Sigma-Aldrich
Ethanol, ACS reagent, prima fine spirit, without additive, F15 o1
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2,6-Lutidine, ReagentPlus®, 98%
Sigma-Aldrich
Methanol, BioReagent, ≥99.93%
Sigma-Aldrich
Methanol, ACS spectrophotometric grade, ≥99.9%