Electrochemical technologies offer new approaches to mitigating carbon emissions associated with energy and chemical processing. While the molecular assembly of ions at electrode-electrolyte interfaces is often thought to play key roles in governing the performance of batteries and other devices, ion assembly at high charge density interfaces remains poorly understood. For example, ionic assembly in concentrated electrolytes is defined by ion-ion interactions and collective behaviors, which are missed by classical mean field theory. Ionic liquids are fluids composed of ions, and studies of “electric double layer” formation in ionic liquids have driven qualitatively new understanding of ionic assembly at charge-ordered interfaces. I will discuss our work aimed at linking nanoscale structures and dynamics of ionic liquid-solid interfaces to electrochemical properties as a model for evaluating how knowledge of collective ionic assembly can guide electrochemical device design. I will highlight our ongoing work bridging surface forces measurements with electrochemical analysis to understand how systematic “doping” of charge imbalances into ionic liquid electrolytes influences interfacial properties. I will conclude by showing how these fundamental studies can be leveraged to enhance capacitance and charge transfer kinetics at electrochemical interfaces to advance energy storage and electrochemical carbon dioxide recycling.

Linking interfacial nanostructure to electrochemical properties in ionic liquids

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ACS Spring 2023

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