Multifunctional Shaped MOF-Biopolymer Composite for Enzymatic Catalysis and Pollutant Removal

Abstract We report a novel strategy for constructing a multifunctional catalytic bioreactor by integrating diverse metal–organic frameworks (MOFs) into gelatin via a green coacervation process. A wide range of chemically stable Zr, Fe, Al, and Ti MOFs were incorporated into the gelatin matrix, forming robust composites with good MOF loadings, high porosity, and crystallinity. In particular, the UiO-66(Zr)/gelatin composite was developed for sustainable catalysis and environmental remediation. These composites could be easily shaped into different forms, including tablets and monoliths. It exhibited high adsorption capacity and selectivity toward cationic dyes such as methylene blue, highlighting its potential for dye removal. This hydrogel composite could also be combined with laccase to form a laccase@UiO-66(Zr)/gelatin composite, which exhibited high catalytic efficiency for the degradation of dyes and the oxidative polymerization of phenolic pollutants under harsh conditions (broad pH, elevated temperatures) and over multiple cycles. The shaped biocatalysts also showed tunable product retention or release depending on the gelatin content. This highlights the high potential of the laccase@UiO-66(Zr)/gelatin composite as a scalable, eco-friendly enzyme-based biocatalytic system with applications in environmental remediation.