Total Synthesis Toolkit for Constructing Multi-Catalytic Colloidal Hybrid Nanoparticles

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Professor Raymond Schaak at the Pennsylvania State University is supported by the Macromolecular, Supramolecular, and Nanochemistry (MSN) program in work to develop a total synthesis framework for the rational construction of complex colloidal hybrid nanoparticles for use in multi-catalytic reaction processes. This research builds on recently established nanoparticle analogues of orthogonal reactivity, site-specific reactivity, chemoselectivity, regiospecificity, substituent effects, and coupling chemistry. The reaction toolkit will be expanded to include new classes of nanoparticle transformations, linear vs. radial growth modes, and protection-deprotection strategies for overcoming the hybrid nanoparticles? natural tendencies toward nucleation and reactivity. Ultimately, these synthetic tools and an understanding of how they occur will expand our knowledge of how to construct exceptionally complex hybrid nanoparticles and how to place nanoparticles at any desired location on a multi-domain particle. These complex colloidal hybrid nanoparticles will be explored for use as multi-catalyst systems that couple several sequential catalytic transformations in a single-pot reaction.Chemists approach the synthesis of large molecules by rationally modifying and linking together smaller molecular building blocks in a stepwise manner. This process, which contrasts sharply with existing design capabilities for inorganic nanostructures, is guided by mechanistic considerations and empirical guidelines and is facilitated by an extensive library of chemical transformations. Colloidal hybrid nanoparticles, which contain multiple distinct nanoparticle domains fused together through solid-state interfaces, can be considered as "artificial molecules." A primary goal of this research is to develop new synthetic tools, along with mechanistic insights into how they work, that will help to bridge the gap between the synthetic capabilities that exist for complex molecules vs. those available for hybrid nanoparticle systems, which are much less advanced. These colloidal hybrid nanoparticles have the potential to function as modular systems for efficiently carrying out multiple catalytic reactions in a single pot. A diverse group of students, including a team of undergraduate researchers, will be exposed to a unique cross-disciplinary project and will actively participate in a variety of outreach efforts. A new inquiry-based undergraduate laboratory module to apply organic synthesis concepts to hybrid nanoparticle systems will be developed, and assignments introducing students to scientific ethics and the interface of chemistry and society will be developed and integrated into freshman chemistry courses.