Metal nanoparticles are found ubiquitously as heterogeneous catalysts for a wide variety of industrial, organic, and energy catalytic processes. The electronic and steric environment at the nanoparticle surface has a huge impact on the reactivity and selectivity of catalytic transformations occurring at surface active sites. In heterogeneous catalysis, the structural knobs that are utilized to tune catalytic behavior include the nanoparticle morphology and composition and the support. All three of these structural changes alter electronic, steric, and ensemble properties in major and mutually convoluted ways. In contrast, molecular catalysis has developed subtle ways to tune the steric and electronic properties of a metal active site, primarily through the ligand sphere. In this work, we demonstrate several ligand-based surface functionalization strategies to tune the catalytic behavior of nanoparticle catalysts. These include 1) the adsorption of inorganic ligands on nanoparticle surfaces in order to synthesize precisely controlled monolayer and sub-monolayer core-shell catalysts, 2) the use of conductive bridging ligands to anchor molecular complexes onto nanoparticle surfaces to tune electronic properties and 3) electrochemical and thermal strategies to generate single atom alloy surfaces. All of these strategies develop new structural frameworks for tuning the surface active site environment in order to access more active and selective nanoparticle catalysts.

Tailoring catalytic ensemble geometry using colloidal nanoparticle-ligand interactions

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.