State-of-the-art technology for cyclohexanone oxime production typically demands elevated temperature and pressure, along with the utilization of expensive hydroxylamine sulfate or oxidants. Here, we propose an electrochemistry-assisted cascade strategy for the efficient cyclohexanone ammoximation under ambient conditions by using in situ cathode-generated green oxidants of reactive oxygen species (ROS) such as OOH* and H 2 O 2 . This electrochemical reaction can take place at the cathode, achieving over 95% yield, 99% selectivity of cyclohexanone oxime, and an electron-to-oxime (ETO) efficiency of 96%. Mechanistic analysis reveals that, in addition to the direct ammoximation by in situ–generated OOH* by electrocatalytic ORR, Ti-MOR also play a major role in capturing OOH* directly and converting the in situ–generated H 2 O 2 to OOH*, thus accelerating the ORR-coupled cascade production of cyclohexanone oxime. This work paves a mild, economical, and sustainable energy-efficient electrocatalytic route for the oxime production using oxygen, ammonium bicarbonate, and cyclohexanone.
25 January 2020 in Angewandte Chemie International Edition
Hydrophobic Sn-Beta zeolites, hydrothermally synthesized via structural reconstruction, exhibit unparalleled catalytic performances for Lewis acid-catalyzed reactions, far outperforming post-synthesized Sn-Beta and state-of-the-art Sn-Beta-F materials.
This study proposes a novel strategy for preparing Ti-Beta zeolite with nanosized crystals and incredibly stable isolated Ti4+ ions under solvent-free conditions via intensified interzeolite transformation from a commercially available Ti-MWW source. The obtained Ti-Beta exhibited unique catalytic performance in the oxidation of cyclohexene with aqueous hydrogen peroxide.