Abstract
Catalytic epoxidation of linear α-olefins (LAOs) through Mukaiyama epoxidation provides a premier route to valorization of these unique valuable materials in the Fischer-Tropsch synthesis crude. However, this reaction suffers a kinetically slow formation of key acyl/acyl peroxy radicals by the metal-based catalysts when using O2 as oxidant, resulting in the lowered overall reaction efficiency. Herein, we report a strategy for rational tuning the electronic properties of transition metal oxides catalyst by modulation of metal-support interaction, which could realize almost perfect yield (99%) of desired epoxides in transformation of 1-decene. Varieties of experimental and theoretical characterizations demonstrate that the superior catalytic performance results from the altered electronic state of active sites, which is closely correlated with the electronic interaction between metal oxide and support. This work greatly advances catalytic epoxidation of long-chain LAOs and paves the road for valorization of FTS crude.
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