CAREER: Rational Design of Dual-Functional Photocatalysts for Synthetic Reactions: Controlling Photosensitization and Reaction with a Single Nanocrystal

With support from the Chemical Catalysis (CAT) program of the NSF Division of Chemistry, Dr. Chen Wang of the Department of Chemistry and Biochemistry at Queens College, City University of New York, is developing novel catalysts based on perovskite nanocrystals for utilizing light to efficiently synthesize organic chemicals that are essential in biomedical and pharmaceutical applications. The project will employ various spectroscopic methods to understand how photo-generated excited states in the nanocrystals can convert light energy and selectively promote the desired chemical processes on the nanocrystal surface. The project integrates synthetic chemistry, physical chemistry, materials science, and instrumentation development and hence will provide a multidisciplinary learning environment for students at all levels. Photochemical research will be introduced into the undergraduate curriculum to train students from diverse cultural backgrounds. Outreach activities, including photochemistry workshops and summer research camps, are planned to reach out to K-12 students and encourage a diverse, talented pool of students to consider pursuing studies in science, technology, engineering and mathematics fields. Photocatalytic synthesis has the potential to provide for streamlined, energy-efficient synthetic routes into useful molecules by providing novel bond construction manifolds. The proposed project will explore catalytic platforms with metal halide perovskite nanocrystals (PNCs) with the goals of achieving both efficient photosensitization and reaction control. The project will engineer the PNC surface will the goal of facilitating important synthetic reactions, such as cycloadditions and C-C coupling reactions, and with the goal of understanding the modified PNC surface through a combination of experimental and computational investigation. Surface photocatalytic processes will be tracked using a variety of ultrafast spectroscopic methods, including transient absorption, time-resolved photoluminescence, and time-resolved stimulated resonance Raman spectroscopy. This mechanistic study aims to reveal the relationship between the surface environment of PNCs and their catalytic performance to guide the rational design of novel photocatalysts based on semiconductor nanocrystals. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.