Catalytic Transfer Hydrogenation of Furfural to Furfuryl Alcohol with Recyclable Al-Zr@Fe Mixed Oxides
Catalytic Transfer Hydrogenation of Furfural to Furfuryl Alcohol with Recyclable Al-Zr@Fe Mixed Oxides
复制标题
可回收Al-Zr@Fe混合氧化物催化转移氢化糠醛制备糠醇
DOI：
10.1002/cctc.201701266
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发表时间：
2018-01-23
期刊：
影响因子：
4.5
通讯作者：
Yang, Song
中科院分区：
文献类型：
--
作者：
He, Jian;Li, Hu;Yang, Song
采用共沉淀法制备了一系列具有磁性的酸/碱双功能Al-Zr@ Fe 3 O 4催化剂，并将其用于以异丙醇为氢源的糠醛催化转移加氢制糠醇反应。采用XRD、N2物理吸附、振动样品磁强计、热重分析、X射线荧光光谱、NH3/CO2程序升温脱附、SEM和TEM等技术对催化剂的物化性能和形貌进行了表征。结果表明，当Al 3 +/Zr 4 +/Fe 3 O 4的摩尔比为21：9：3时，催化剂在180 ℃下反应4 h，糠醇收率可达90.5%，活化能较低，为45.3kJmol（-1）。此外，浸出和可再循环性测试证实了Al7Zr3@Fe3O4（1/1）作为非均相催化剂起作用，其可以重复用于至少五个连续的反应运行，而在通过外部磁体简单回收后催化活性没有显著损失。值得注意的是，该催化剂被证明对于其他生物质衍生的呋喃醛的氢化也是有效的。
A series of magnetic, acid/base bifunctional Al-Zr@Fe3O4 catalysts were successfully prepared by a facile coprecipitation method and utilized in the catalytic transfer hydrogenation (CTH) of furfural to furfuryl alcohol with 2-propanol as hydrogen source. The physicochemical properties and morphologies of the as-prepared catalysts were characterized by various techniques, including XRD analysis, N-2 physisorption, vibrating sample magnetometry, thermal gravimetry analysis, X-ray fluorescence spectroscopy, NH3/CO2 temperature-programmed desorption, SEM, and TEM. The Al7Zr3@Fe3O4(1/1) catalyst with a Al3+/Zr4+/Fe3O4 molar ratio of 21:9:3 was found to exhibit a high furfuryl alcohol yield of 90.5% in the CTH from furfural at 180 degrees C after 4h with a comparatively low activation energy of 45.3kJmol(-1), as calculated from the Arrhenius equation. Moreover, leaching and recyclability tests confirmed Al7Zr3@Fe3O4(1/1) to function as a heterogeneous catalyst that could be reused for at least five consecutive reaction runs without significant loss of catalytic activity after simple recovery by an external magnet. Notably, the catalyst proved also efficient for hydrogenation of other biomass-derived furanic aldehydes.