Microfluidic paper-based analytical devices (μPADs) have experienced an unprecedented story of success. In particular, as of today, most people have likely come into contact with one of their two most famous examplesthe pregnancy or the SARS-CoV-2 antigen test. However, their sensing performance is constrained by the optical readout of nanoparticle agglomeration, which typically allows only qualitative measurements. In contrast, single-impact electrochemistry offers the possibility to quantify species concentrations beyond the pM range by resolving collisions of individual species on a microelectrode. Within this work, we investigate the integration of stochastic sensing into a μPAD design by combining a wax-patterned microchannel with a microelectrode array to detect silver nanoparticles (AgNPs) by their oxidative dissolution. In doing so, we demonstrate the possibility to resolve individual nanoparticle collisions in a reference-on-chip configuration. To simulate a lateral flow architecture, we flush previously dried AgNPs along a microchannel toward the electrode array, where we are able to record nanoparticle impacts. Consequently, single-impact electrochemistry poses a promising candidate to extend the limits of lateral flow-based sensors beyond current applications toward a fast and reliable detection of very dilute species on site.
During the recent SARS-CoV-2 pandemic, lateral flow assays (LFAs) have written an indescribable story of success, as they provide means for decentralized, low-cost, and easy-to-use testing. However, LFAs in their most common form support only qualitative results and their sensitivity and limit of detection is significantly limited by the colorimetric readout method. In contrast, single-impact electrochemistry offers the possibility to quantify species beyond picomolar concentrations by recording individual species collisions with a biased microelectrode. Within this work, we investigate the integration of stochastic sensing into a LFA-architecture by combining a wax-patterned microchannel with a microelectrode array in order to detect silver nanoparticles by their oxidative dissolution. Here, we demonstrate the possibility to resolve individual nanoparticle collisions in a paper-based microchannel using a simplified reference-on-chip setup. Furthermore, we simulated a lateral-flow sensor, by flushing previously dried silver nanoparticles towards the electrode array, where the particles are subsequently detected. This proof-of-principle illustrates that single-impact electrochemistry might be a promising technique to extend the capability of LFAs. Especially, the integration of functionalized nanoparticle labels could enable the rapid and on-site detection of very dilute species with exceptional sensitivity.
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