ChemCatChem
Gas-phase enzymatic catalysis offers great potential for both green synthesis and the efficient degradation of volatile chemicals. However, solid enzymes often exhibit extremely low activity compared to their counterparts in native aqueous phase. While a few immobilization methods have succeeded in increasing activity by preserving enzyme structure, approaches...
Employing enzymatic reaction cascade principles to synthesize artificial materials with multiple autonomously operating active sites is one of the holy grails in modern catalysis research. In this regard, metal-organic frameworks (MOFs) are promising host platforms. Yet, applying MOFs as enzyme-mimicking catalysts is synthetically challenging. Herein,...
It has been a long-standing goal for chemists to develop selective catalytic oxidation systems with molecular oxygen as a green terminal oxidant from the inspiration of active sites in natural metalloenzymes. Lanthanide-centered methanol dehydrogenase (Ln-MDH), which contained the same pyrroloquinoline quinone (PQQ) redox cofactor as the analogous calcium-based...
Installing fluoroalkyl motifs into biorelevent indoles is particularly interesting due to their ubiquitous presence in drug molecules. Herein, we demonstrate the regioselective C4 fluoroalkoxylation of indoles using fluoroalcohols via palladium-catalyzed chelation-assisted C–H activation. The weak chelating benzoyl moiety at the C3 position acts as...
Copper complexes supported by thio- and selenoether ligands provide a coordination environment similar to the active sites of methionine-containing copper monooxygenases. Spectroscopic data, supported by theoretical studies, suggest that the chalcogenoethers act as hemilabile ligands, providing access to electrophilic side-on cupric–superoxo intermediates...
In this work, we employed flame spray pyrolysis (FSP), a high-temperature synthesis method, to control the formation of Pd structures on the CeO2 support. Multiple types of Pd structures deposited on CeO2 are observed on FSP-made samples. Our results show that the oxidizing environment during FSP synthesis facilitates the formation of incorporated Pd2+ structures,...
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