2026-09-26T09:03:10Z https://www.ideals.illinois.edu/oai-pmh

oai:www.ideals.illinois.edu:2142/115644 2023-07-11 col_2142_5131 col_2142_14789 com_2142_5130 com_2142_14788 com_2142_8903

Rodríguez-López, Joaquín Rodríguez-López, Joaquín Murphy, Catherine Jain, Prashant K Han, Hee-Sun 2022-05 application/pdf en text Submission published under a 24 month embargo labeled 'U of I Access', the embargo will last until 2024-05-01 The student, Kendrich Hatfield, accepted the attached license on 2022-04-20 at 13:17. The student, Kendrich Hatfield, submitted this Dissertation for approval on 2022-04-20 at 13:58. This Dissertation was approved for publication on 2022-04-21 at 16:40. DSpace SAF Submission Ingestion Package generated from Vireo submission #17848 on 2022-11-14 at 00:24:50 Electrochemical and spectroelectrochemical investigations of interfacial electrode processes Hatfield, Kendrich O'Donaghue 2022-04-21 Electrochemistry Surface-enhanced Raman spectroscopy Scanning Electrochemical Microscopy Thin film electrodes Electrode interfaces are critical players in the development of medical, industrial, and energy-related technologies and a thorough understanding of the surface electrochemistry is required to design better devices and materials. Analytical methods for studying electrode surfaces in situ vary widely and give information ranging from chemical speciation to electron transfer properties. Electrochemical methods using the analyte of interest as the working electrode provide vital interfacial properties such as kinetics, mass transport, and thermodynamics of electrode processes across the entire interface. In this dissertation, such techniques are shown to determine the charge transport properties and mechanisms of a redox-active solid thin film, successfully applying redox polymer theory to model how charge transport is affected by redox dopant loading. To investigate local structural changes at interfaces, this dissertation explores the incorporation of surface-enhanced Raman spectroscopy (SERS) to electroanalytical experiments. I demonstrate the viability of scanning electrochemical microscopy (SECM) to control local surface pH at a self-assembled monolayer and SERS to track the resulting structures. To broaden the application of electrochemical SERS to carbon-based electrodes, I demonstrate a hybrid nanoparticle-graphene substrate and use it to characterize the electrochemical reduction of anthraquinone-2,6-disulfonate on graphene. Further, I show the capability of SECM to induce SERS-detectable changes at these carbon substrates and suggest further possible research directions for this and other projects using coupled Raman-SECM. Overall, this work demonstrates several new methods for deeper fundamental understanding of complex electrode interfaces, probing charge transport, local solution perturbation effects, and adsorption chemistry. Thesis eng https://hdl.handle.net/2142/115644 Copyright 2022 Kendrich Hatfield Ph.D. Dissertation Chemistry University of Illinois at Urbana-Champaign Chemistry