Self-adjusted reaction pathway enables efficient oxidation of aromatic C-H bonds over zeolite-encaged single-site cobalt catalyst
The selective oxidation of aromatic C-H bonds to high value-added oxygenated products with mo-lecular oxygen remains a key challenge in heterogeneous catalysis.Eligible heterogeneous catalysts are pursued and the reaction mechanism is hotly debated.Herein,we report that zeolite-encaged single-site cobalt ions can efficiently catalyze the model reaction of ethylbenzene aerobic oxidation to acetophenone,outperforming the industrial benchmark catalyst cobalt naphthenate under iden-tical conditions.The self-accelerating phenomenon is observed in the progress of ethylbenzene aerobic oxidation,corresponding to the self-adjusted reaction pathway as revealed by kinetic stud-ies and density functional theory calculations.The formation of reactive O* species on Co sites,re-sembling the well-known α-O on Fe sites,is identified to be responsible for the self-adjusted reac-tion pathway of aromatic C-H bond oxidation.
C-H bonds activationHeterogeneous catalysisCo@Y zeoliteSelf-acceleratingReactive O* species
党健、李玮杰、秦斌、柴玉超、武光军、李兰冬
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南开大学化学学院,有机新物质创造前沿科学中心,天津 300071
南开大学材料科学与工程学院,天津 300350
碳-氢键活化 多相催化 Co@Y分子筛催化剂 自加速 活性氧物种
Fundamental Research Funds for the Central Universities(Nankai University).国家自然科学基金Fundamental Research Funds for the Central Universities(Nankai University).国家自然科学基金Fundamental Research Funds for the Central Universities(Nankai University).国家自然科学基金中央高校基本科研业务费专项南开大学项目
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