Design and synthesis of metal organic frameworks for CO₂ separation and catalysis
Description
TitleDesign and synthesis of metal organic frameworks for CO₂ separation and catalysis
Date Created2013
Other Date2013-10 (degree)
Extentxxi, 144 p. : ill.
DescriptionEnergy demand is currently a prevalent global issue that we are facing due to the dramatic increase in both population and industrial processes around the world. Presently, over 80% of the world's energy consumption is supplied by the burning of non-renewable fossil fuels. The CO₂ gas emitted from this process has proven to contribute to global warming. One possible strategy in addressing this problem is the development of materials that can selectively capture CO₂ from flue gas mixtures. A new flexible microporous metal-organic framework (MMOF), [Zn2(bpdc)2(bpe)]·2DMF (bpdc = 4,4'- biphenyldicarboxylate, bpe = 1,2-bis(4-pyridyl)-ethane, DMF = N,N- dimethylformamide), was synthesized and found to selectively capture CO2 over other small gasses (N₂, CH₄, O₂ and CO), which makes it good candidate for CO₂ separation. Another possible method to solve the energy crisis is to find an alternative, clean and renewable energy source/carrier, such as hydrogen, to replace traditional fossil fuels. Recently, scientists have proposed that producing hydrogen from the water splitting process is an efficient and reliable way to create this clean burning fuel due to the high abundance of water sources on earth. Water oxidation is considered to be the bottleneck of the whole reaction due to the thermodynamic and kinetic limitations, hence development of materials that can catalyze water oxidation is then highly desired. A previously reported Mn based MOF, [Mn₄(μ₃-OMe)(nic)₄] (nic = isonicotinate), was synthesized and was found to form birnessite-type MnO₂ nanoparticles during the photochemical water oxidation reaction, which is known to be an efficient heterogeneous water oxidation catalyst. In addition to water oxidation, MOFs can also be used as heterogeneous catalysts for other organic transformations, with the active sites either integrated at metal nodes or located on the backbones of the frameworks. A new layered MOF structure, [Co(Hoba)₂(H2O)₂] (H₂oba = 4,4'-oxydibenzoic acid), was synthesized and, after removal of the terminal water molecules, was found to be a highly active heterogeneous catalyst for olefin epoxidation with both high conversion and selectivity to form epoxide products. Finally, synthesis, characterization, PL properties and preliminary results of gas adsorption studies of a new MOF are described.
NotePh.D.
NoteIncludes bibliographical references
Noteby Jingming Zhang
Genretheses, ETD doctoral
Languageeng
CollectionGraduate School - New Brunswick Electronic Theses and Dissertations
Organization NameRutgers, The State University of New Jersey
RightsThe author owns the copyright to this work.
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