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

Autor: Yang F; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France.; College of Chemistry and Chemical Engineering, Yantai University, 264005, Yantai, China., Rousselot-Pailley P; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Nicoletti C; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Simaan AJ; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Faure B; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Courvoisier-Dezord E; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Amouric A; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Charmasson Y; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Backov R; Université de Bordeaux, CNRS, CRPP, UMR5031, 115 Avenue Albert Schweitzer, 33600, Pessac, France., Tron T; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France., Mekmouche Y; Aix Marseille Univ, Centrale Marseille CNRS, iSm2, 13397, Marseille, France.
Jazyk: angličtina
Zdroj: ChemPlusChem [Chempluschem] 2023 May; Vol. 88 (5), pp. e202300156.
DOI: 10.1002/cplu.202300156
Abstrakt: 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⊂UNIK 157 ) or opposite position (1⊂UNIK 71 ) 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⊂UNIK 157 being twice as active than 1⊂UNIK 71 (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.
(© 2023 The Authors. ChemPlusChem published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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