UiO‐66 and hcp UiO‐66 Catalysts Synthesized from Ionic Liquids as Linker Precursors
UiO‐66 and hcp UiO‐66 Catalysts Synthesized from Ionic Liquids as Linker Precursors
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DOI：
10.1002/open.202000291
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发表时间：
2020-12-16
期刊：
影响因子：
2.3
通讯作者：
Hartmann M
中科院分区：
文献类型：
--
作者：
Ermer M;Mehler J;Rosenberger B;Fischer M;Schulz PS;Hartmann M
使用离子液体（IL）作为连接体前体，已经成功地合成和表征了众所周知的金属有机框架（MOF）UiO-66（Universitetet i奥斯陆）和最近报道的MOF hcp UiO-66（六方密堆积）。由于IL的溶解性更好，所应用的新合成方法的优点是经济和环境友好的后处理程序。此外，与对苯二甲酸相比，对苯二甲酸根阴离子的反应性增加，导致MOF形成更快，MOF结构中的缺陷量增加。以香茅醛环化合成异蒲勒醇为实验反应，考察了缺陷对催化性能的影响。hcp UiO-66和fcc UiO-66（面心立方）的活性与其他基于MOF或沸石的催化剂相比有所改善，而选择性相似。 使用离子液体作为金属有机框架hcp和fcc UiO-66合成的连接体前体可导致更快的结晶，从而减少合成时间和消耗的能量。此外，由于骨架内的缺陷，在香茅醛环化成异蒲勒醇中的MOFs的催化活性增加，而选择性不受影响。
Using ionic liquids (ILs) as linker precursors, the well‐known metal‐organic framework (MOF) UiO‐66 (Universitetet i Oslo) and the recently reported MOF hcp UiO‐66 (hexagonal closed packed) have been successfully synthesized and characterized. The advantage of the applied novel synthesis approach is an economically and environmentally benign work‐up procedure, due to the better solubility of the IL. Additionally, the reactivity of the terephthalate anions is increased compared to terephthalic acid, resulting in faster MOF formation with an increased amount of defects in the MOF structure. In order to explore to the influence of defects on the catalytic performance, the cyclisation of citronellal to isopulegol was employed as test reaction. The activity of hcp UiO‐66 and fcc UiO‐66 (face centered cubic) is improved compared to other MOF or zeolite based catalysts, while the selectivity is similar. The use of ionic liquids as linker precursor for the synthesis of the metal‐organic frameworks hcp and fcc UiO‐66 results in faster crystallization thereby reducing synthesis time and energy consumed. Furthermore, the catalytic activity of the MOFs in the cyclization of citronellal to isopulegol is increased due to defects within the frameworks while the selectivity is not affected.
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