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Author Contact: djudd@wesleyan.edu
Local Identifier: 1683"},{"label":"Author-supplied Keywords","value":["Infrared spectroscopy","Catalysis","Shape reconfiguration","Plasmon-mediated synthesis","Inorganic chemistry","Nanoparticles"]},{"label":"Degree","value":["Master of Arts"]},{"label":"Description","value":"

Nanoparticles offer a level of synthetic customization unique to materials of their size. The inherent flexibility in and control over particle morphology and composition situate these materials as optimal surfaces for active and selective catalysis. Monometallic silver (Ag) nanoparticles can change shape and internal defect structure solely through light illumination. The associated localized surface plasmon resonance (LSPR) that occurs at the surface of the nanoparticle drives citrate oxidation and facilitates Ag+ reduction. This oxidation is also sensitive to pH and the concentration of Ag+ ions and other shape-directing precursors. Interconversion between particle architectures improves Ag nanoparticle recyclability and diversifies the shape-dependent functionalities a single solution can assume. The optimization of a shape reconfiguration pathway, with prisms transforming into icosahedra and etched spheres before returning to their original state, required balancing competing kinetic and plasmonic variables. Essential alterations to the previously developed procedure included increasing the intensity of the incident 550 nm light and raising the pH of the final growth solution. Characterization techniques, such as scanning electron microscopy (SEM), UV-Vis spectroscopy, and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) helped connect particle morphology to its optical behavior and elucidated surface coverage of residual adsorbates on supported catalysts following their synthesis. DRIFTS experimentation focused on establishing baselines for common compounds in Ag particle syntheses and extending the in situ capabilities of the instrument, with the ultimate goal aimed at observing reaction dynamics and surface adsorbates over elevated temperatures. Characterization extended beyond the Ag particles produced by plasmon-mediated methodologies to include gold (Au) concave cubes produced by Ag underpotential deposition. Building a new gas flow system and establishing a procedure for in situ DRIFTS investigations promotes future work on the surface dynamics of catalytic reaction pathways and other associated chemicals

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