Departamento de Nuevas Arquitecturas en Química de Materiales - Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC) , Sor Juana Inés de la Cruz 3, Cantoblanco 28049, Madrid, Spain.
J Am Chem Soc. 2016 Jul 27;138(29):9089-92. doi: 10.1021/jacs.6b05706. Epub 2016 Jul 15.
With the aim of developing new highly porous, heterogeneous Lewis acid catalysts for multicomponent reactions, a new mesoporous metal-organic framework, InPF-110 ([In3O(btb)2(HCOO)(L)], (H3btb = 1,3,5-tris(4-carboxyphenyl)benzene acid, L = methanol, water, or ethanol), has been prepared with indium as the metal center. It exhibits a Langmuir surface area of 1470 m(2) g(-1), and its structure consists of hexagonal pores with a 2.8 nm aperture, which allows the diffusion of multiple substrates. This material presents a large density of active metal sites resulting in outstanding catalytic activity in the formation of substituted α-aminonitriles through the one-pot Strecker reaction of ketones. In this respect, InPF-110 stands out compared to other catalysts for this reaction due to the small catalyst loadings required, and without the need for heat or solvents. Furthermore, X-ray single crystal diffraction studies clearly show the framework-substrate interaction through coordination to the accessible indium sites.
为了开发用于多组分反应的新型高多孔、多相路易斯酸催化剂,我们制备了一种新型介孔金属有机骨架材料 InPF-110([In3O(btb)2(HCOO)(L)],(H3btb=1,3,5-三(4-羧基苯基)苯酸,L=甲醇、水或乙醇),其中铟为金属中心。该材料具有 1470 m(2)g(-1)的 Langmuir 比表面积,其结构由具有 2.8nm 孔径的六方孔组成,允许多种底物扩散。该材料具有大量的活性金属位点,在酮的一锅法斯特克反应形成取代的α-氨基腈中表现出优异的催化活性。在这方面,与其他用于该反应的催化剂相比,InPF-110 的突出之处在于所需的催化剂负载量较小,并且不需要加热或溶剂。此外,X 射线单晶衍射研究清楚地表明了通过与可及的铟位点配位的骨架-底物相互作用。