Cu/SiO2 synthesized with HKUST-1 as precursor: high ratio of Cu+/(Cu+ + Cu0) and rich oxygen defects for efficient catalytic hydrogenation of furfural to 2-methyl furan.
Cu/SiO2 synthesized with HKUST-1 as precursor: high ratio of Cu+/(Cu+ + Cu0) and rich oxygen defects for efficient catalytic hydrogenation of furfural to 2-methyl furan.
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DOI：
10.1039/d3cp02806b
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发表时间：
2023-09
期刊：
影响因子：
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通讯作者：
Zhiyuan Zong;Hongzi Tan;Pengrui Zhang;Chao Yuan;Rongrong Zhao;Feng Song;Weiming Yi;Fengshan Zha
中科院分区：
文献类型：
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作者：
Zhiyuan Zong;Hongzi Tan;Pengrui Zhang;Chao Yuan;Rongrong Zhao;Feng Song;Weiming Yi;Fengshan Zha
Cu/SiO2催化剂是糠醛加氢反应最有前途的催化剂之一，但其结构和表面性质难以调控。在此，我们开发了一种MOF衍生的Cu/SiO2催化剂（Cu/SiO2-MOF）用于FF加氢制2-甲基呋喃（2-MF）。与蒸氨法（Cu/SiO2-AE）和传统浸渍法（Cu/SiO2-TI）相比，Cu/SiO2-MOF中的铜物种不仅通过Cu-O-Si键固定在SiO2表面，而且暴露出更多的活性中心。通过这种方式，通过强的金属-载体相互作用构建了更高的Cu+/（Cu+ + Cu 0）比和更丰富的氧缺陷，这是导致上级催化性能的原因。此外，还发现溶剂效应对产物分布的影响对2-MF和环戊酮（CPO）的选择性起着重要的调节作用。本研究不仅为深入了解Cu/SiO2-MOF催化FF加氢反应的机理提供了理论依据，而且为其他多相催化领域高效催化剂的设计和合成提供了参考。
Cu/SiO2 is one of the most promising catalysts for the furfural (FF) hydrogenation reaction but suffers from the difficulty of tailoring the microstructure and surface properties. Herein, we developed a MOF-derived Cu/SiO2 catalyst (Cu/SiO2-MOF) for FF hydrogenation to 2-methyl furan (2-MF). In comparison with Cu/SiO2 catalysts prepared from ammonia evaporation (Cu/SiO2-AE) and traditional impregnation (Cu/SiO2-TI), the copper species in Cu/SiO2-MOF could not only be anchored on the silica surface via forming Cu-O-Si bonds but also exposed many more active sites. In this way, a higher ratio of Cu+/(Cu+ + Cu0) and richer oxygen defects were constructed via strong metal-support interactions, which were responsible for the superior catalytic performance. In addition, it was found that the solvent effect on product distribution played an important role in adjusting the selectivity to 2-MF and cyclopentanone (CPO). The present work not only provides a deep insight into the catalytic mechanism of Cu/SiO2-MOF for the FF hydrogenation reaction but also sheds light on the design and synthesis of highly efficient catalysts for other heterogeneous catalysis fields.