期刊
JOURNAL OF CATALYSIS
卷 286, 期 -, 页码 266-272出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2011.11.011
关键词
Catechol oxidase; Biomimetic; Flow; Heterogeneous catalysis; Copper complex; Diazonium salts; Graphite felt; N-tripodal ligand
The catecholase activity of a copper(II) complex coordinated by a tripodal pyrazole-based ligand was investigated in continuous flow catalysis. The covalent immobilization of the complex on the surface was achieved by a two steps method. First, the porous graphite felt support is functionalized by electrochemical reduction of 4-carboxymethyl-benzenediazonium salts. Second, the complex is covalently immobilized by esterification reaction between the COOH-containing linker and a primary alcohol group present on the C6 chain of the ligand. The two steps of the immobilization process were optimized by using nitro-containing molecules and cyclic voltammetry analyses. The copper complex exhibits higher catecholase activity in continuous flow catalysis than in solution with a 50 times lower amount of catalyst, underlining the advantages of the flow procedure. The presence of H2O2 is detected after catalysis, showing that the four-electron reduction of dioxygen to water does not occur unlike the natural enzyme. (C) 2011 Elsevier Inc. All rights reserved.
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