Date of Award
John B. Wiley
Hydrogen fuel is one of the most important areas of research in the field of renewable energy development and production. Hydrogen gas can be generated by fuel cells, water electrolyzers, and heterogeneous nanoscale catalysts. It can be burned to directly release chemical energy or condensed for storage and transport, providing fuel for combustion devices or storing excess energy generated by renewable sources such as wind turbines and concentrated solar power assemblies. While platinum is the most active catalyst for hydrogen reduction, its high cost significantly deters its utilization in advanced photocatalytic materials. One approach to mitigating this expense is optimizing the morphology and placement of nanostructured platinum catalysts. Highly crystalline, morphologically-controlled platinum nanoparticles (Pt NPs) have been effectively utilized to increase hydrogen generation efficiency in a variety of nanocomposite materials. However, synthesis routes to high-quality Pt NPs can be dangerous and difficult to replicate. Furthermore, utilization of the Pt NPs in nanocomposite materials is hindered by lack of control over catalyst placement.
Nanopeapods are versatile nanocomposites that offer a high degree of control over catalyst placement as well as the potential for interesting new properties arising from the interaction between the catalyst and a semiconductor. Platinum@hexaniobate nanopeapods (Pt@HNB NPPs) consist of linear arrays of Pt NPs encapsulated within the scrolled semiconductor hexaniobate. Pt@HNB NPPs offer significant advantages over similar composites by utilizing the isolated reduction environment of the encapsulated Pt NP arrays to decrease kinetic competition and surface crowding.
This work describes the design, fabrication, and implementation of the new nanocomposite platinum@hexaniobate nanopeapods for sensitized hydrogen production under visible light irradiation. The following chapters present facile microwave heating syntheses of highly crystalline Pt nanocubes and Pt@HNB NPPs with consistent morphology and high catalyst loading. A detailed study is also presented of the optical properties of the Pt nanocubes, which produced a UV-range absorbance band that indicates the formation of a localized surface plasmon resonance. Most significantly, preliminary results from visible light photolysis indicate that sensitized Pt@HNB NPPs produce hydrogen in quantities comparable to published systems, and that alteration of experimental parameters may result in even greater yields.
Davis-Wheeler Chin, Clare, "Platinum@Hexaniobate Nanopeapods: Sensitized Composite Architectures for Photocatalytic Hydrogen Evolution Under Visible Light Irradiation" (2018). University of New Orleans Theses and Dissertations. 2503.