Redox-Responsive Hydrogen-Bonding Systems for Supramolecular Applications

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Inspired by the iconic example of DNA, which is composed of two strands of natural polymers that are held together by weak forces and can be separated when desired, Professor Smith of San Diego State University explores novel approaches to controlling the reversible assembly and separation of synthetic polymer strands. Such polymeric materials offer the potential for correction of defects and stimuli-responsive properties. In addition to the potential for significant impact in responsive materials, supramolecular polymers and switches, this research program provides excellent education and training opportunities to a diverse group of undergraduate and graduate students, many of whom are from groups under-represented in science. This research project encourages students to decipher what is happening at the molecular level - sharpening their chemical reasoning and problem solving abilities. These abilities are valuable in their future careers. The overall goal of this project is to develop the chemistry of redox-active, linear hydrogen-bond dimers such that binding strength can be strongly, but reversibly, perturbed by electrochemical reduction/oxidation. This research program is broken into three specific aims. Aim 1 is to establish the significance of two electrons and one proton (H+) verse one electron transfer for strongly perturbing hydrogen bonding by comparing the voltammetric behavior of these two types of systems. Aim 2 is to develop new redox-active hydrogen bond dimers in which proton transfer across a hydrogen bond is purposely used to amplify the effect of electron transfer in such a way that binding strength is either greatly increased or decreased. Finally, in Aim 3, the research team explores the use of the redox-active arrays developed to create redox-responsive, supramolecular, polymeric systems.