A serious challenge in photocatalytic solar fuel production lies in the design of efficient catalysts that are stable, have visible light response and are easy to make. In order to realize this goal, efforts should be focused on designing new photocatalysts that have such properties to drive the field forward towards commercialization. Metal-Organic Frameworks (MOFs) are a class of crystalline and porous materials that offer tunable and diverse structural and electronic properties that can be exploited for enhanced photocatalytic solar fuels production. This thesis focuses on the utilization and characterization of a 3-D MOF photocatalyst with metal-oxo chain and pyrene-based ligand as secondary building units. Specifically, through hydrothermal synthesis technique, we constructed a bimetallic cerium/titanium MOF that exhibits excellent and stable photoactivity for visible-light driven hydrogen generation. The incorporation of two redox active metals of CeIII /CeIV and TiIII/TiIV in an oxo-chain connected by a photosensitizing organic ligand resulted in a strong ligand-tometal charge transfer (LMTC), evident by EPR, for efficient reduction of water. A high hydrogen production rate of 49 μmol h-1 was achieved, which is attributed to energetic LMTC and better charge separation. This work expands on MOFs photocatalysis field and open new direction towards designing redox active heterometallic MOFs for solar fuels production.
| Identifer | oai:union.ndltd.org:kaust.edu.sa/oai:repository.kaust.edu.sa:10754/670345 |
| Date | 07 1900 |
| Creators | Alfaraidi, Abdulrahman M. |
| Contributors | Gascon, Jorge, Physical Science and Engineering (PSE) Division, Mohammed, Omar F., Alshareef, Husam N. |
| Source Sets | King Abdullah University of Science and Technology |
| Language | English |
| Detected Language | English |
| Type | Thesis |
| Rights | 2024-07-28, At the time of archiving, the student author of this thesis opted to temporarily restrict access to it. The full text of this thesis will become available to the public after the expiration of the embargo on 2024-07-28. |
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