Enzyme-Based Hybrid Macroporous Foams as Highly Efficient Biocatalysts Obtained through Integrative Chemistry

Abstract

Integrative chemistry-based rational design has been used to synthesize the first lipase [C-CRl]@Glymo-Si(HIPE) and [C-TAl]@Glymo-Si(HIPE) hybrid macrocellular biocatalysts, where immobilization of crude enzymes is optimized, while circumventing the reactants’ low kinetic diffusion, by the use of silica macroporous hosts. As a direct consequence, these new hybrid biocatalysts display unprecedented cycling catalysis performance, as demonstrated by the syntheses of butyloleate ester (used as biodiesel lubricant), hydrolysis of linoleic-glycero ester derivatives (end products used for detergent and soap generations), and trans-esterification (reaction involved in the synthesis of low viscosity biodiesel). Considering that the catalytic performances are given in terms of absolute conversion percentage and not just relative enzyme activity, the enzyme@Glymo-Si(HIPE) hybrid macrocellular biocatalysts presented in this study display unprecedented high yield cycling catalysis performances, where turnover numbers (TON) and turnover frequencies (TOF) show promise for real industrial applications. This study can be considered as a milestone for enzyme-based heterogeneous catalyzes, thereby enhancing their competitiveness with the supported-catalysts commonly used in industry, in total agreement with current sustainable development issues. Also, the new macrocellular biocatalysts are well-suited for large-scale industrial production because of their above-mentioned performance characteristics, further enhanced by their monolithic character, which eases the separation of the catalysts from other reaction components.