Janus electrochemistry: Simultaneous electrochemical detection at multiple working conditions in a paper-based analytical device

Abstract

The simultaneous detection of multiple analytes from a single sample is a critical tool for the analysis of real world samples. However, this is challenging to accomplish in the field by current electroanalytical techniques, where tuning assay conditions towards a target analyte often results in poor selectivity and sensitivity for other species in the mixture. In this work, an electrochemical paper-based analytical device (ePAD) capable of performing simultaneous electrochemical experiments in different solution conditions on a single sample was developed for the first time. We refer to the system as a Janus-ePAD after the two-faced Greek god because of the ability of the device to perform electrochemistry on the same sample under differing solution conditions at the same time with a single potentiostat. In a Janus-ePAD, a sample wicks down two channels from a single inlet towards two discreet reagent zones that adjust solution conditions, such as pH, before flow termination in two electrochemical detection zones. These zones feature independent working electrodes and shared reference and counter electrodes, facilitating simultaneous detection of multiple species at each species' optimal solution condition. The device utility and applicability are demonstrated through the simultaneous detection of two biologically relevant species (norepinephrine and serotonin) and a common enzymatic assay product (p-aminophenol) at two different solution pH conditions. Janus-ePADs show great promise as an inexpensive and broadly applicable platform which can reduce the complexity and/or number of steps required in multiplexed analysis, while also operating under the optimized conditions of each species present in a mixture.

Keywords: Electrochemistry; Janus; Microfluidic paper-based analytical device; Paper-based analytical device.