Freestanding 3D-interconnected carbon nanofibers as high-performance transducers in miniaturized electrochemical sensors.

3D-carbon nanomaterials have proven to be high-performance transducers in electrochemical sensors but their integration into miniaturized devices is challenging. Herein, we develop printable freestanding laser-induced carbon nanofibers (f-LCNFs) with outstanding analytical performance that furthermore can easily allow such miniaturization through a paper-based microfluidic strategy. The f-LCNF electrodes were generated from electrospun polyimide nanofibers and one-step laser carbonization. A three-electrode system made of f-LCNFs exhibited a limit of detection (LOD) as low as 1 nM (S/N = 8) for anodic stripping analysis of silver ions, exhibiting the peak at ca. 100 mV vs f-LCNFs RE, without the need of stirring. The as-described system was implemented in miniaturized devices via wax-based printing, in which their electroanalytical performance was characterized for both outer- and inner-sphere redox markers and then applied to the detection of dopamine (the peak appeared at ca. 200 mV vs f-LCNFs RE) with a remarkable LOD of 55 pM. When modified with Nafion, the f-LCNFs were highly selective to dopamine even against high concentrations of uric and ascorbic acids. Especially the integration into closed microfluidic systems highlights the strength 3D porous structures provides excellent analytical performance paving the way for their translation to affordable lab-on-a-chip devices where mass-production capability, unsophisticated fabrication techniques, transfer-free, and customized electrode designs can be realized.

Integrating high-performing electrochemical transducers in lateral flow assay.

Lateral flow assays (LFAs) are the best-performing and best-known point-of-care tests worldwide. Over the last decade, they have experienced an increasing interest by researchers towards improving their analytical performance while maintaining their robust assay platform. Commercially, visual and optical detection strategies dominate, but it is especially the research on integrating electrochemical (EC) approaches that may have a chance to significantly improve an LFA's performance that is needed in order to detect analytes reliably at lower concentrations than currently possible. In fact, EC-LFAs offer advantages in terms of quantitative determination, low-cost, high sensitivity, and even simple, label-free strategies. Here, the various configurations of EC-LFAs published are summarized and critically evaluated. In short, most of them rely on applying conventional transducers, e.g., screen-printed electrode, to ensure reliability of the assay, and additional advances are afforded by the beneficial features of nanomaterials. It is predicted that these will be further implemented in EC-LFAs as high-performance transducers. Considering the low cost of point-of-care devices, it becomes even more important to also identify strategies that efficiently integrate nanomaterials into EC-LFAs in a high-throughput manner while maintaining their favorable analytical performance. Graphical abstract.

Flow-Through Carbon Nanofiber-Based Transducer for Inline Electrochemical Detection in Paper-Based Analytical Devices.

Point-of-care (POC) devices are rapid, simple, portable, inexpensive, and convenient, but typically they only deliver qualitative results when used in the form of a lateral flow assay (LFA). Electrochemical detection could improve their sensitivity and ensure quantitative detection; however, a breakthrough in material-based technology is needed. We demonstrate a new concept in which electrodes are directly embedded within the lateral flow, enabling flow-through and hence interaction with the entire sample. This is accomplished through laser-induced carbon nanofibers (LCNFs) made by electrospinning Matrimid into nanofiber mats with subsequent pyrolyzing of electrode structures through a CO2 laser. Their highly porous 3D structure and superior graphene-like electrochemical properties are ideally suited for flow-through electrochemical LFA (EC-LFA), where the LCNFs are simply added in line with the other membranes. After optimization of the setup, biological binding assays typical for LFA diagnostics were successfully implemented, enabling the highly sensitive and quantitative detection of 137 pM DNA target sequences of a pathogenic organism that rivals the performance of pump-controlled microfluidic bioassays. This demonstrates that LCNF-based transducers can transform paper-based diagnostic tests to enable precise, quantitative analysis without reliance on cost-intensive read-out systems.