Synthesis Modulation as a Tool To Increase the Catalytic Activity of Metal-Organic Frameworks: The Unique Case of UiO-66(Zr)
Synthesis Modulation as a Tool To Increase the Catalytic Activity of Metal-Organic Frameworks: The Unique Case of UiO-66(Zr)
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DOI：
10.1021/ja405078u
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发表时间：
2013-08-07
影响因子：
15
通讯作者：
De Vos, Dirk E.
中科院分区：
文献类型：
--
作者：
Vermoortele, Frederik;Bueken, Bart;De Vos, Dirk E.
对苯二甲酸锆U10 -66（Zr）的催化活性可以通过使用调制方法而显著增加。在合成过程中，三氟乙酸和HCl的组合使用产生高度结晶的材料，其中三氟乙酸盐部分取代了三氟乙酸盐。材料的热活化不仅导致六核Zr簇的脱羟基化，而且还导致合成后去除三氟乙酸酯基团，从而导致具有大量开放位点的更开放的框架。因此，该材料是几种刘易斯酸催化反应的高活性催化剂。
The catalytic activity of the zirconium terephthalate UiO-66(Zr) can be drastically increased by using a modulation approach. The combined use of trifluoroacetic acid and HCl during the synthesis results in a highly crystalline material, with partial substitution of terephthalates by trifluoroacetate. Thermal activation of the material leads not only to dehydroxylation of the hexanuclear Zr cluster but also to post-synthetic removal of the trifluoroacetate groups, resulting in a more open framework with a large number of open sites. Consequently, the material is a highly active catalyst for several Lewis acid catalyzed reactions.