Analytical electrochemistry at supramolecular interfaces: structural probing and dynamic sensing

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Electrochemistry has regained popularity in the last two decades, not only with the ever-growing demand of designing clean and renewable energy conversion devices (e.g., modern batteries, fuel cells, and solar panels), but also with the motivation of developing point-of-care electrochemical biosensors (beyond hand-held glucose meters). We are interested in adapting electrochemical principles and techniques to evaluate molecular interfaces in order to investigate how molecules assemble and interact at solid-liquid interfaces. The goal of the proposed research program is to expand the capabilities of analytical electrochemistry as a routine and powerful tool for probing and modulating the molecular environment at electrified interfaces.******It is challenging to create high performance electrochemical devices given the multidisciplinary nature of this task, particularly the construction of ideal electrode-electrolyte interfaces with catalytic or sensing molecules assembled with optimized coverage, distribution, and orientation. In complement to microscopic imaging techniques based on advanced instrumentation, our approach is to adapt supramolecular chemistry for building and examining electrified molecular interfaces. A class of pumpkin-shape, nanometer-size host molecules have been recently synthesized and found to recognize electroactive guest molecules through noncovalent, reversible binding with ultrahigh affinity (superior to antibody-antigen interaction). The assembly of these rather large host molecules on the surface tethered with guest ligands can be sensed by conventional electrochemical measurements, and provide accurate measures of available space and locations of the surface. Subsequently, we will study how to modulate the interfacial formation of supramolecular inclusion complex, in order to create dynamic surfaces for applications not limited to biosensing.******The proposed research offers an interdisciplinary platform for the training of highly qualified personnel; electrochemists, analytical chemists, biochemists, and synthetic chemists will work together with both the fundamental science and potential applications in mind. The success of the proposed research will put Canada in a leading position in adapting supramolecular chemistry for analytical electrochemistry studies and applications thereof. *****