Organometallic Functionalization of Colloidal Nanocrystal Surfaces for Catalysis

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With the support of the Chemical Catalysis program in the Division of Chemistry, Emily Tsui of the University of Notre Dame will study new ways of using light to accelerate important chemical transformations. Nanomaterials with semiconductor properties have long been studied for light-induced chemical transformations. However, the precise measurement and control of the surface properties of these materials for chemical reactivity are difficult to achieve experimentally. The project will focus on using metal centers attached to light-absorbing nanoparticles to provide information about the properties of the nanoparticles, and to act as reaction centers for important catalytic transformations such as carbon-carbon bond formation reactions. The results obtained from these studies will guide the development of new light-promoted reactions. This grant will also support the research training of graduate and undergraduate students in this interdisciplinary field. Professor Tsui’s research team will actively participate in outreach activities involving local elementary school students, with a focus on developing educational modules on nanomaterials-based chemistry. Educational videos on practical topics in electrochemistry and catalysis will also be produced by the graduate students and Dr. Tsui, and will made freely available online to the general public.In these studies Emily Tsui and her team at the University of Notre Dame will study the use of organometallic metal carbonyl fragments coordinated to the surfaces of semiconductor nanocrystal quantum dots for photocatalytic reactions. Quantum dots have been targeted as photosensitizers and photocatalysts for many reactions due to their tunable light-absorbing properties, but many questions remain regarding the effects of surface chemistry upon these transformations. The Tsui group will explore the use of surface-bound metal carbonyl fragments to act as spectroscopic reporters of quantum dot surface effects including the surface dipole moment, which can correlate to photocatalytically-relevant properties such as band edge potentials. The development of a quantitative model of these spectroscopic features is expected to lead to a more detailed understanding of how surface effects contribute to quantum dot reactivity during photoredox transformations. Additionally, Dr. Tsui will study the use of the surface-bound organometallic fragments to act as catalytic centers during photocatalytic transformations. Graduate students will be trained in both organometallic chemistry and materials characterization methods, providing them interdisciplinary experience that will be professionally valuable. These students will also be trained in scientific communication through participation in outreach activities and in the preparation of a series of electrochemistry videos that will be disseminated online.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.