Using Nanomaterials to Solve Environmental Problems: Advancing the Science and Engineering of Photocatalysis
Brame, Jonathon Andrew
Alvarez, Pedro J.
Doctor of Philosophy
Photocatalysis is a process by which materials can transfer light energy into chemical energy in the form of reactive oxygen species (ROS), which can then oxidize chemical and biological contaminants in water. Whereas photocatalysis offers the potential to treat many recalcitrant priority pollutants in a cost-effective manner, it has yet to become a viable, wide-spread treatment option due to implementation barriers that include limitations in treatment efficiency and relatively high costs of some photocatalytic material. This thesis seeks to increase the applicability and understanding of nanomaterial-enhanced photocatalytic oxidation processes to help overcome these barriers. Increased photocatalytic efficiency can be accomplished through informed choice of ROS-producing materials. For example, hydroxyl radicals are shown to be much more susceptible to hindrance by natural organic matter (NOM), phosphate and wastewater treatment plant effluent than 1O2, which is only slightly inhibited by NOM and not by phosphate or wastewater effluent. Additionally, a novel crystallization mechanism for photocatalytic TiO2 nanotubes enabled photo-production of multiple ROS types. This “cocktail” of reactive oxygen species contributed to increased efficiency. Novel applications for nanotechnology-enhanced photocatalysis were demonstrated at the lab scale. These include (1) photocatalytic pre-treatment of weathered oil from the 2010 Gulf oil spill, which increased soluble organic carbon content (indicative of increased bioavailability) by 60% and enhanced subsequent biodegradation by 37%; and (2) a water disinfection case study in rural Swaziland, which produced a prototype fluidized bed photoreactor capable of removing 99.9% of bacteria and viruses in <60 seconds. These projects show both a variety of applications for photocatalysis, and ways to increase its efficiency and effectiveness. To achieve wide-spread implementation, however, the price of photocatalysis must be reduced. Extensive reuse of treatment materials (>60 cycles), and utilization of less-purified starting materials (>90% cost reduction) highlight possible ways to reduce the cost of nanomaterial photocatalysis. By reducing financial implementation barriers, defining niches where photocatalysis can be superiorly effective, engineering reactor systems that enable real-world testing of this technology, and increasing understanding of photocatalytic inhibition mechanisms, photocatalysis can become a tool to help solve global water challenges.
Nanomaterials; Nanotechnology; Photocatalyst; Water treatment