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Design, Synthesis, Stability, and Photocatalytic Studies of Sustainable Metal-Organic Frameworks

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Date Issued:
2018
Abstract/Description:
The presented dissertation focuses on the design, synthesis, and characterization of metal-organic frameworks (MOFs) composed of earth-abundant elements the exhibit photoredox activity and studied their application as heterogeneous photocatalysts in organic synthesis and in solar-to-chemical energy conversion. In particular, the structure-property relationships of titanium-based MOFs relating the structure of the organic building unit and the photophysical and photochemical activity of the solid material is studied. The first novel family of seven MOFs isoreticular to MIL-125-NH2, includes functionalized with N-alkyl groups with increasing chain length (methyl to heptyl) and with varying connectivity (primary or secondary). The functionalized materials displayed reduced optical bandgaps correlated with the increased inductive donor ability of the alkyl substituents, enhanced excited-state lifetimes, mechanistic information towards visible light CO2 reduction, and improved water stability. The second family of titanium MOFs was prepared with a new secondary building unit and organic links of varying lengths, for which Their crystal structure was solved utilizing powder X-ray diffraction crystallography. This work provides guidelines for the next generation of photocatalyst for the conversion of solar-to-chemical energy and other organic transformations.
Title: Design, Synthesis, Stability, and Photocatalytic Studies of Sustainable Metal-Organic Frameworks.
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Name(s): Logan, Matthew, Author
Uribe Romo, Fernando, Committee Chair
Zhai, Lei, Committee Member
Yuan, Yu, Committee Member
Kuebler, Stephen, Committee Member
Rahman, Talat, Committee Member
University of Central Florida, Degree Grantor
Type of Resource: text
Date Issued: 2018
Publisher: University of Central Florida
Language(s): English
Abstract/Description: The presented dissertation focuses on the design, synthesis, and characterization of metal-organic frameworks (MOFs) composed of earth-abundant elements the exhibit photoredox activity and studied their application as heterogeneous photocatalysts in organic synthesis and in solar-to-chemical energy conversion. In particular, the structure-property relationships of titanium-based MOFs relating the structure of the organic building unit and the photophysical and photochemical activity of the solid material is studied. The first novel family of seven MOFs isoreticular to MIL-125-NH2, includes functionalized with N-alkyl groups with increasing chain length (methyl to heptyl) and with varying connectivity (primary or secondary). The functionalized materials displayed reduced optical bandgaps correlated with the increased inductive donor ability of the alkyl substituents, enhanced excited-state lifetimes, mechanistic information towards visible light CO2 reduction, and improved water stability. The second family of titanium MOFs was prepared with a new secondary building unit and organic links of varying lengths, for which Their crystal structure was solved utilizing powder X-ray diffraction crystallography. This work provides guidelines for the next generation of photocatalyst for the conversion of solar-to-chemical energy and other organic transformations.
Identifier: CFE0007219 (IID), ucf:52217 (fedora)
Note(s): 2018-08-01
Ph.D.
Sciences, Chemistry
Doctoral
This record was generated from author submitted information.
Subject(s): Metal-organic frameworks -- MOFs -- photocatalysis -- photoredox -- synthesis -- characterization -- earth-abundant -- sustainable -- solid-state -- applied materials -- crystallography -- organic -- inorganic
Persistent Link to This Record: http://purl.flvc.org/ucf/fd/CFE0007219
Restrictions on Access: public 2018-08-15
Host Institution: UCF

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