Metal Organic Frameworks as Solid Acid Catalysts for Acetalization of Aldehydes with Methanol
Metal Organic Frameworks as Solid Acid Catalysts for Acetalization of Aldehydes with Methanol
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DOI：
10.1002/adsc.201000537
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发表时间：
2010-11-22
影响因子：
5.4
通讯作者：
Garcia, Hermenegildo
中科院分区：
文献类型：
--
作者：
Dhakshinamoorthy, Amarajothi;Alvaro, Mercedes;Garcia, Hermenegildo
以金属有机骨架（MOFs）为固体多相催化剂，研究了室温下醛与甲醇的缩醛化反应。在测试的MOF中，含铜的MOF [Cu-3（BTC）（2）]（BTC = 1，3，5-苯三羧酸酯）显示出比含铁的MOF [Fe（BTC）]和含铝的MOF [Al-2（BDC）（3）]（BDC= 1，4-苯二羧酸酯）更好的催化活性。该方案被验证为一系列的芳香族和脂肪族醛，并用于保护各种醛到商业上重要的缩醛，在良好的产率，而不需要除去水。此外，该催化体系的重复使用性和多相性也得到了证实。通过粉末X射线衍射、Brunauer-Emmett-Teller表面积测量和用于转化大量苯甲醛的失活催化剂的傅立叶变换红外光谱分析表征，进一步研究了MOF的结构稳定性。铜MOF作为缩醛化催化剂的性能与其它常规的均相和多相催化剂如氯化锌、沸石和粘土的性能相比是有利的。
Room temperature acetalization of aldehydes with methanol has been carried out using metal organic frameworks (MOFs) as solid heterogeneous catalysts. Of the MOFs tested, a copper-containing MOF [Cu-3(BTC)(2)] (BTC = 1,3,5-benzenetricarboxylate) showed better catalytic activity than an iron-containing MOF [Fe(BTC)] and an aluminium containing MOF [Al-2(BDC)(3)] (BDC=1,4-benzenedicarboxylate). The protocol was validated for a series of aromatic and aliphatic aldehydes and used to protect various aldehydes into commercially important acetals in good yields without the need of water removal. In addition, the reusability and heterogeneity of this catalytic system was demonstrated. The structural stability of MOF was further studied by characterization with powder X-ray diffraction, Brunauer-Emmett-Teller surface area measurements and Fourier-transformed infrared spectroscopic analysis of a deactivated catalyst used to convert a large amount of benzaldehyde. The performance of copper MOF as acetalization catalyst compares favourably with those of other conventional homogeneous and heterogeneous catalysts such as zinc chloride, zeolite and clay.