Abstract

A non-faradaic label-free cortisol biosensor was demonstrated using MoS2 nanosheets integrated into a nanoporous flexible electrode system. Low volume (1–5 μL) sensing was achieved through use of a novel sensor stack design comprised of vertically aligned metal electrodes confining semi-conductive MoS2 nanosheets. The MoS2 nanosheets were surface functionalized with cortisol antibodies towards developing an affinity biosensor specific to the physiological relevant range of cortisol (8.16 to 141.7 ng/mL) in perspired human sweat. Sensing was achieved by measuring impedance changes associated with cortisol binding along the MoS2 nanosheet interface using electrochemical impedance spectroscopy. The sensor demonstrated a dynamic range from 1–500 ng/mL with a limit of detection of 1 ng/mL. A specificity study was conducted using a metabolite expressed in human sweat, Ethyl Glucuronide. Continuous dosing studies were performed during which the sensor was able to discriminate between four cortisol concentration ranges (0.5, 5, 50, 500 ng/mL) for a 3+ hour duration. Translatability of the sensor was shown with a portable form factor device, demonstrating a comparable dynamic range and limit of detection for the sensor. The device demonstrated a R2 correlation value of 0.998 when comparing measurements to the reported impedance values of the benchtop instrumentation.

Highlights

  • Wearable diagnostic biosensors for the detection and monitoring of analytes in transdermal sweat present an intriguing pathway toward improving user health outcomes in an inexpensive and noninvasive manner[1]

  • Once cortisol molecule binds to antibody, the surface charge becomes less negative (Fig. 3c). These results suggest that the cortisol antigens have bound to the cortisol antibodies immobilized onto the MoS2 nanosheet surface and show a dose dependent electrochemical response across the pH range typical of human sweat

  • Detection of cortisol in physiologically relevant ranges of perspired human sweat was demonstrated at low volume (1–5 μL) using a vertically-aligned metal electrode sensor system in conjunction with confined semi-conductive MoS2 nanosheets

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Summary

Introduction

Wearable diagnostic biosensors for the detection and monitoring of analytes in transdermal sweat present an intriguing pathway toward improving user health outcomes in an inexpensive and noninvasive manner[1]. Cortisol is released in response to stress and low blood-glucose concentration It functions to increase blood sugar through gluconeogenesis, suppress the immune system, and aid in the metabolism of fat, protein, and carbohydrates[11] while decreasing bone formation[12]. This allows for the prospect of using relative changes in cortisol expression as a means of monitoring a potentially immuno-compromised state[13,14,15,16,17]. To detect relative deviations in the body’s natural fluctuations, a dynamic determination of cortisol levels is needed without the use of costly and cumbersome laboratory equipment

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