Investigating the binding interaction of nanoparticles with small molecules using solution nuclear magnetic resonance
Date
2023-05
Authors
DiLorenzo, Yeongseo An
Major Professor
Advisor
Venditti, Vincenzo
Huang, Wenyu
Rossini, Aaron
Sadow, Aaron
VanVeller, Brett
Committee Member
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Abstract
Nanoparticle (NP) catalysts have found various applications in many different fields. Since NP catalysis is a surface-based process, characterizing dynamic processes occurring at the NP surface is critical for engineering new and more efficient catalysts and nanomaterials. However, our understanding of the structural, kinetics, and thermodynamics of the sorption equilibria is limited due to a lack of experimental techniques that allow us to obtain such information reliably at atomic resolution. In recent years, solution nuclear resonance (NMR) spectroscopy has emerged as a preferred tool to investigate small molecule-NP interactions. Indeed, due to its ability to probe dynamic processes occurring over a wide range of timescales with atomic resolution, NMR spectroscopy is applicable to various small molecule-NP systems and can provide a comprehensive characterization of the sorption equilibria involving multiple adsorbed species and intermediate states.
The studies presented in this dissertation demonstrate using solution NMR methods to investigate small molecule-NP interactions. Specifically, this dissertation illustrates the characterization of the adsorption of phenolic compounds onto the surface of ceria-supported palladium (Pd/CeO2) nanorods using the increase in the 13C transverse relaxation rate upon the addition of NPs (13C ΔR2). Moreover, this dissertation reports the library of organogels based on low molecular-mass organic gelators (LMOGs) that can stabilize NP suspensions in various organic solvents to prepare stable NMR samples containing NPs. Finally, this dissertation shows how the combined analysis of multiple solution NMR methods can be used to investigate the substrate-support interaction between phenol and palladium supported on titania (Pd/TiO2) NPs.
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dissertation