Chemi-Impeditive Sensing Platform Based on Single-Walled Carbon Nanotubes

Chemical sensing methodology based on electrochemical impedance spectroscopy (EIS) targeting analytes in aqueous samples on functionalized single-walled carbon nanotube (SWCNT) is reported. The SWCNT in contact with electrolyte shows unique impedance spectra that cannot be analyzed with classical equivalent circuit models. Inspired by the charge transport property of mixed ionic-electronic conductors, we propose an equivalent circuit based on transmission line model (TLM), by which the impedance of the CNT-electrolyte system can be analyzed to track down all the equivalent circuit parameters. By combining multiple pieces of information, which are technically immeasurable with conventional chemiresistive or chemicapacitive techniques, several analyte species responding to the sensor can be differentiated from each other. We demonstrate the "chemi-impeditive" concept on chemically modified SWCNTs for detecting perfluoroalkyl substances (PFAS) in aqueous solutions. The EIS coupled with a fluorination chemistry on SWCNT surface provides unique changes in equivalent circuit components for each PFAS, i.e., changes in CNT and solution resistances, as well as interfacial CNT-solution capacitance, through which perfluorooctanesulfonic acid, perfluorooctanoic acid, hexafluoropropylene oxide dimer acid, and perfluorobutanesulfonic acid are detected in a discriminative manner. The new impedimetric method opens up new vistas in chemical sensing in that the EIS analysis provides an additional dimension of information beyond the single resistance or capacitance typically measured by many conventional types of sensors.