Local Microenvironments at Disordered Interfaces Visualized through Ensemble Measurements
Jillian Dempsey a
a University of North Carolina at Chapel Hill, Department of Chemistry, Chapel Hill, Carolina del Norte 27599, EE. UU., Chapel Hill, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2021 (NFM21)
#SolCat21. (Photo-)Electrocatalysis: From the Atomistic to System Scale
Online, Spain, 2021 October 18th - 22nd
Organizers: Karen Chan, Sophia Haussener and Brian Seger
Invited Speaker, Jillian Dempsey, presentation 167
DOI: https://doi.org/10.29363/nanoge.nfm.2021.167
Publication date: 23rd September 2021

Disorder in real materials influences their properties and the chemical processes that occur at their interfaces. In order to unravel, and ultimately control processes at these interfaces, it is essential to gain a molecular-level understanding of the underlying physical manifestations caused by disordered materials. To accomplish this, measurement techniques through which disorder can be detected, quantified, and monitored are needed. However, such quantitative measurements are notoriously difficult, as effects often average out in ensemble measurements. In our lab, we have employed a combination of electrochemical and spatially resolved surface spectroscopy measurements to illuminate a molecular-level picture of disorder in materials. We study amorphous carbon which is an intrinsically disordered material. To the amorphous carbon, we covalently attached a monolayer of ferrocene. Interfacial electron transfer across the amorphous carbon–ferrocene interface is highly sensitive to the local microenvironment felt by the ferrocene, and thus to disruptions of order. By systematically varying linker properties and surface loadings, the influence of lateral interactions between nonuniformly distributed ferrocene headgroups on ensemble electrochemical measurements is gleaned.

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