Controlled Immobilization of a Palladium Complex/Laccase Hybrid into a Macrocellular Siliceous Host

Fangfang Yang (1, 2) , Pierre Rousselot-Pailley (1) , Cendrine Nicoletti (1) , A. Jalila Simaan (1) , Bruno Faure (1) , Elise Courvoisier-Dezord (1) , Agnès Amouric (1) , Yolande Charmasson (1) , Rénal Backov (3) , Thierry Tron (1) , Yasmina Mekmouche (1)

1 ISM2 - Institut des Sciences Moléculaires de Marseille
2 YTU - Yantai University
3 CRPP - Centre de Recherche Paul Pascal

This study investigates the site-directed immobilization of a hybrid catalyst bearing a biquinoline-based-Pd(II) complex (1) and a robust laccase within cavities of a silica foam to favor veratryl alcohol oxidation. We performed the grafting of 1 at a unique surface located lysine of two laccase variants, either at closed (1⊂UNIK157) or opposite position (1⊂UNIK71) of the enzyme oxidation site. After immobilization into the cavities of silica monoliths bearing hierarchical porosity, we show that catalytic activity is dependent on the orientation and loading of each hybrid, 1⊂UNIK157 being twice as active than 1⊂UNIK71 (203 TON vs 100 TON) when operating under continuous flow. These systems can be reused 5 times, with an operational activity remaining as high as 40 %. We show that the synergy between 1 and laccase can be tuned within the foam. This work is a proof of concept for controlling the organization of a heterogeneous hybrid catalyst using a Pd/laccase/silica foam

Domaines: Catalyse; Chimie de coordination; Chimie organique

Fangfang Yang, Pierre Rousselot-Pailley, Cendrine Nicoletti, A. Jalila Simaan, Bruno Faure, et al.. Controlled Immobilization of a Palladium Complex/Laccase Hybrid into a Macrocellular Siliceous Host. ChemPlusChem, 2023, 88 (5), pp.e202300156. ⟨10.1002/cplu.202300156⟩. ⟨hal-04105029⟩