Author

Zixin Wang

Date of Award

Summer 2022

Document Type

Open Access Dissertation

Department

Chemistry and Biochemistry

First Advisor

Hui Wang

Abstract

Nanoparticles of platinum group elements(Pd, Pt, Rh, Ir, Ru and Os) exhibit intriguing catalytic behaviors that are sensitively dependent upon their particle dimensions, chemical compositions, and surface structures. Platinum group elementbased nanomaterials have been widely utilized for catalyzing a series of important chemical reactions, producing over 90% of chemicals and fuels and accounting for 35% of the world's GDP globally. Reducing the overall particle sizes of the catalysts to the sub-10 nm size regime not only effectively mitigates the cost issues associated with the noble metal-based materials, but also remarkably modifies the surface atomic coordinations and the electronic band energies, both of which may profoundly influence the catalytic behaviors of the catalysts. To prevent particle sintering and agglomeration during catalytic reactions, these sub-10 nm metal nanocatalysts are typically dispersed on solid state support materials with high surface areas. Here, we use a bioinspired polymer, polydopamine, and its carbonized derivative, N-doped carbon, as easily processible colloidal support materials for sub-10 nm platinum group metal nanocatalysts with precisely controlled particle sizes, narrow size distributions, ligand-free clean surfaces, and highly uniform dispersion on the support surfaces. Taking full advantage of the precise control over the particle sizes, morphologies, and crystalline phases, we have been able to establish detailed correlations between the nanocatalyst structures and the molecular transforming behaviors on the catalyst surfaces.

Available for download on Saturday, October 05, 2024

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