초록 |
Epoxides have been regarded as pivotal ingredients for manufacturing pesticides, aerosols, resins, and other chemical products. Currently adopted epoxidation methods exhibit relatively low selectivity, harsh reaction conditions, limited olefin substrates scope, and risk of explosion issues. It would be essential to exploit sustainable methodologies to address the above-mentioned disadvantages and achieve commercial-scale synthesis. Herein, we report electrocatalytic epoxidation via the generation of Co-oxo intermediate in Co-TAML molecular catalysts. High valent metal-oxo species have been considered as active oxidants for oxygen atom transfer (OAT) reactions. Without additional oxidants, it can epoxidize olefin substrates using water as a sole oxygen atom source at ambient conditions. According to “oxo-wall theory,” terminal oxo ligands on late transition metal beyond ‘group 8’ are known to form weak metal-oxo bonds owing to the increasing occupancy of anti-bonding metal d-orbitals. We tried to characterize Co-TAML oxo intermediates with cyclic voltammetry and spectroelectrochemical studies. |