We are interested in the design and construction of nanostructured architectures that couple molecular transport (analyte/reagent delivery), chemical sensing (optical or electrochemical) and subsequent chemical processing withinin the same physical construct.  The ultimate goal of these experiments is to produce chemical reagents in situ and consume them directly at a proximal reaction site, all within the confined geometry of a low-dimensional nanostructure, so that chemical transformations may be realized with optimal efficiency.  To realize this goal we are developing sensing strategies that efficiently match electron transfer and spectroscopic probing to low-dimensional, i.e. zero- and one-dimensional nanostructures. As one example, vertically-oriented nanopores provide fluidic communication in nanocapillary array membranes supporting embedded annular nanoband electrodes (EANEs) fabricated on the interior of the nanopores.  In these structures, electroosmotic flow (EOF) is used to enhance the delivery of electroactive species to the EANE, and the same potential used to achieve EOF also drives electron transfer.  Because transport and electron transfer are intimately coupled, high efficiency conversions are achieved. The efficiency of electrochemical treatment is improved to near 100% efficiency compared to diffusion-limited efficiencies of 5-10% in microfluidic structures.

High efficiency coupling of chemical sensing to chemical treatment in low-dimensional nanofluidic structures

248th National Meeting (2014)

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