In Situ-Induced Synthesis of Magnetic Cu-CuFe2O4@HKUST-1 Heterostructures with Enhanced Catalytic Performance for Selective Aerobic Benzylic C–H Oxidation

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• 作者：Shuang Fan ; Wenjun Dong ; Xiubing Huang ; Hongyi Gao ; Jingjing Wang ; Zhaokui Jin ; Jia Tang ; Ge Wang
• 刊名：ACS Catalysis
• 出版年：2017
• 出版时间：January 6, 2017
• 年：2017
• 卷：7
• 期：1
• 页码：243-249
• 全文大小：478K
• ISSN：2155-5435

文摘

The multifunctional design of heterogeneous catalysts which can realize the selective oxidation of C–H bonds with oxygen at low temperature is of crucial importance in the catalysis community. Here, we report the designed synthesis of Cu-CuFe₂O₄@HKUST-1 heterostructures that is highly active for the selective oxidation of benzylic C–H bonds under mild conditions (60 °C). In the synthetic process, the Cu(0) component of Cu-CuFe₂O₄ nanoparticles gradually released Cu²⁺ ions which were in situ transformed into the HKUST-1 shell. The high activity can be attributed to a rationally multifunctional design of Cu-CuFe₂O₄@HKUST-1 heterostructures, in which Cu-CuFe₂O₄ can provide multiple active sites while HKUST-1 attracts and preconcentrates molecular oxygen. Notably, the catalytic performance under optimized reaction conditions (60 °C) was achieved in the oxidation of fluorene to fluorenone (conversion: > 99%, selectivity: > 99%). Furthermore, the Cu-CuFe₂O₄@HKUST-1 catalyst could be easily recovered by magnetic separation and reused for 10 times without significant loss of catalytic activity.