Bipolar electrochemistry for enrichment, separations, and membraneless electrochemically mediated desalination

Knust, Kyle Nicholas
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Developments in bipolar electrochemistry for the simultaneous separation and enrichment of charged species and membraneless electrochemically mediated desalination (EMD) are presented. Each of these techniques requires an electrochemically generated local electric field within a microchannel and control over bulk fluid flow. In addition to bipolar electrochemical studies, investigations of ion depletion zone formation and EMD in a two-electrode microelectrochemical cell are presented. The dual-channel bipolar electrode (BPE) configuration is employed for the simultaneous enrichment and separation of anions and cations within a single microchannel at an ion depletion zone generated by buffer neutralization. Moreover, this experimental design is also used to generate an ion depletion zone and associated electric field gradient by Cl⁻ oxidation, where we demonstrate partial seawater desalination without the need for a physical membrane. Expanding upon the fundamentals of BPE focusing, we demonstrate proof-of-concept biomolecule separation and enrichment. Moreover, without the need for a direct external electrical connection, one hundred BPEs are operated simultaneously in parallel to enrich multiple analyte bands. Metal deposition at a BPE is used to mediate BPE focusing. Ion depletion zones arising from Cl⁻ oxidation are investigated by making axial electric field measurements while varying key experimental parameters affecting ion depletion zone formation, location, and strength. We investigate the capabilities of EMD by modifying the electrode design to increase the local electric field strength in an effort to increase the percentage of salt rejection. We also examine the possibility to lower, or even eliminate the electrical energy requirements of EMD by driving Cl⁻ oxidation photoelectrochemically. Lastly, on-line capacitively coupled contactless conductivity measurements are presented to rapidly and reliably quantify ion separation for EMD.