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 size, the nanoparticle composition, and the support identity. All three of these structural changes will alter electronic, steric, and other ensemble properties in drastic 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 strategies to alter the catalytic behavior of nanoparticle catalysts. In the first strategy, we utilize the adsorption of inorganic ligands on nanoparticle surfaces in order to synthesize precisely controlled monolayer and sub-monolayer core-shell catalysts. In the second strategy, we utilize conductive bridging ligands to anchor molecular complexes onto nanoparticle surfaces in order to control the electronics and speciation of active metals. Finally, in the third strategy, we use colloidal deposition followed by electrochemical or thermal treatment to generate single atom alloy surfaces. All of these strategies develop new structural frameworks for tuning the surface ligand environment in order to access more active and selective nanoparticle catalysts.

Tailoring the surface of metal nanoparticles for selective electrocatalysis

2019 Fall National Meeting

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