Multifunctional Framework Materials for Catalysis, Chiral Resolution, and Gas Separation

Date
2014
Authors
Li, Peng
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Abstract

New heterogeneous catalysts with greater reusability, efficiency, and ease of synthesis are continuously sought for environmental concerns. Micro/mesoporous materials have been extensively studied for their high internal surface area where the pore/channel catalytic sites lead to improved efficiency. Metal−organic frameworks (MOFs) are crystalline hybrid solids composed of organic struts and inorganic nodes and have emerged as a novel class of porous materials. Thanks to their catalysis friendly features such as large surface areas and porosity, tunable and functionalizable pore walls, MOFs have more advantages to be a kind of heterogeneous catalyst than traditional organic and inorganic porous materials.

As an alternative to traditional porous materials, hydrogen-bonded organic framework materials (HOFs) have some advantages such as solution processability and characterization, easy purification, and straightforward regeneration and reusage by simple recrystallization over porous MOF materials, some porous HOF materials might be potentially implemented in the industrial and/or pharmaceutical applications.

This dissertation project have focused on developing multifunctional porous framework materials (including MOFs and HOFs materials) for their potential application in heterogeneous catalysis, chiral resolution, and gas separations.

One project is about developing a series of sulfonate-based Metal-organic framework materials (MOFs) for use as heterogeneous catalysts for the production of important pharmacological N-containing heterocycles organic compounds. My investigations led to several new efficient heterogeneous catalyst, which are named as Zn-MOF, Cd-MOF, and Cu-MOF. These MOFs are further examined for different catalytic systems, such as Biginelli reactions, Multifunctional pyridine derivatives, and 1,2,3-triazole compounds. These MOFs catalysts not only show good to excellent yield for the organic transformation of N-containing heterocycles organic compounds, but also can be easily recycled to reuse by simple filtration without significant loss of catalystic activities.

In the second project, three HOFs (HOF-2, HOF-3, and HOF-4) have been designed and synthesized and their structures have been characterized by single-crystal diffraction determination techniques. Because of the different structural features of these HOFs, they are used to target various functionalities, such as chiral resolution, acetylene purification, and C2 hydrocarbons separations. Though the developmnet of HOF materials is still in the early stage. The realization of differernt functionality in these HOF materials demonstrate the potential for development HOF materials as a new class of functional porous framework materials for practical applications.

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Keywords
chiral resolution, gas adsorption, gas separation, heterogeneous catalysis, hydrogen-bonded organic framework, metal-organic framework
Citation
Department
Chemistry