Combining a Genetically Engineered Oxidase with Hydrogen-Bonded Organic Frameworks (HOFs) for Highly Efficient Biocomposites

Wied, P; Carraro, F; Bolivar, JM; Doonan, CJ; Falcaro, P; Nidetzky, B

Abstract

Enzymes incorporated into hydrogen-bonded organic frameworks (HOFs) via bottom-up synthesis are promising biocomposites for applications in catalysis and sensing. Here, we explored synthetic incorporation of d-amino acid oxidase (DAAO) with the metal-free tetraamidine/tetracarboxylate-based BioHOF-1 in water. N-terminal enzyme fusion with the positively charged module Z(basic2) strongly boosted the loading (2.5-fold; approximate to 500 mg enzyme g(material)(-1)) and the specific activity (6.5-fold; 23 U mg(-1)). The DAAO@BioHOF-1 composites showed superior activity with respect to every reported carrier for the same enzyme and excellent stability during catalyst recycling. Further, extension to other enzymes, including cytochrome P450 BM3 (used in the production of high-value oxyfunctionalized compounds), points to the versatility of genetic engineering as a strategy for the preparation of biohybrid systems with unprecedented properties.

Keywords: Biocatalysis; Hydrogen-Bonded Organic Frameworks; Immobilization; Metal-Organic Frameworks; Porous Carrier

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Hydrogen-bonded Organic Framework (HOF) Materials

HOF (Hydrogen-Bonded Organic Framework) materials are composed of organic molecules that are connected to each other through hydrogen bonds to form a crystal structure with specific structure and properties. These materials have potential applications in the field of drug delivery, especially in drug entrapment and release. The macropores and channel structures of HOF materials can be used to accommodate drug molecules. Therefore, they can be used as potential drug embedding carriers to help improve the stability and solubility of drugs.

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