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Chemoenzymatic Combination of Glucose Oxidase with Titanium Silicalite‐1

The use and integration of heterogeneous chemical catalysis and biocatalysis, especially using enzymes, will become increasingly important in a future chemical industry based on renewable resources. A range of alternative renewable chemical platforms have already been proposed from biomass, and compared to the conventional fossil-based platform these are radically different. The main difference lies in the high degree of oxyfunctionality of sugar molecules and (poly)alcohols compared to the low functionality of hydrocarbons and aromatics derived from crude oil. Consequently, the approaches for converting these alternative platforms are not identical. In conventional oil-based chemistry, functionality is introduced, whereas functionality should either be removed or used selectively when working with a renewable platform. Furthermore, biomass is usually in the solid form and the inherent oxyfunctionality renders it difficult, if not impossible, to use existing processes to convert the renewable platform into useful chemicals, because it is not easily handled in the gas phase. Therefore, the conversion of biomass will necessarily be carried out in the liquid (aqueous) phase. For the aforementioned reasons, there is now a need to develop a new generation of catalysts, which are able to facilitate the conversion of especially biomass-derived resources in the next generation of chemical processes. It will therefore be advantageous to combine the high stereo-, regio-, and chemoselectivity of enzymes with the diversity, tolerance, and ability of chemical catalysts to operate under various conditions and transform various substrates. In this way the advantages of each catalyst system may be exploited. 5] Additionally these advantages can be integrated and in some cases combined in heterogeneous one-pot reactions with enzymes or even using enzymes linked to the chemical catalyst to further intensify the process and to facilitate catalyst recycling and separation. One such system is the combination of oxidase enzymes with hydrogen peroxide-active titanium silicalite-1 (TS-1—a redox-active molecular sieve with MFI framework). Oxidases (E.C. 1.1.3) provide a useful catalytic approach to selective oxidation under mild conditions using air as a safe oxidant. They are probably more useful than oxygenases, given the need for expensive cofactors, which need to be recycled, when using the latter. This suggested combination has several advantages: