4.8 Article

Nano gold-doped molecularly imprinted electrochemical sensor for rapid and ultrasensitive cortisol detection

Journal

BIOSENSORS & BIOELECTRONICS
Volume 206, Issue -, Pages -

Publisher

ELSEVIER ADVANCED TECHNOLOGY
DOI: 10.1016/j.bios.2022.114142

Keywords

Molecularly imprinted polymer; Electropolymerization; Steroid hormones; Stress marker; Salivary cortisol; Electrochemical sensor

Funding

  1. National Science Foundation [1810067, NNCI-2025489]
  2. National Institutes of Health [1R21DE027170-01]
  3. Oregon State University

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In this study, a molecularly imprinted polymer (MIP)-based electrochemical sensor with enhanced sensitivity for the detection of cortisol was developed. The sensor utilized a nano gold-doped poly-o-PD film, which facilitated charge transfer and blocked the charge transfer when cortisol occupied the binding cavities, resulting in enhanced detection response and sensitivity. The sensor exhibited high affinity and selectivity towards cortisol and showed promising potential for point-of-care testing applications.
Rapid and sensitive detection of steroid hormone cortisol can benefit the diagnosis of diseases related to adrenal gland disorders and chronic stress. We report a molecularly imprinted polymer (MIP)-based electrochemical sensor that utilized nano gold-doped poly o-phenylenediamine (poly-o-PD) film to selectively determine trace level cortisol with enhanced sensitivity. The sensor detected cortisol levels by measuring the current change of the redox-active probes in response to the binding of target cortisol to the imprinted sites in the polymer. The gold-doped MIP (Au@MIP) sensor was prepared using a facile one-step in situ gold reduction and electro-polymerization method to distribute high-density gold nanoparticles in the vicinity of the binding cavities. The in situ gold reduction promote the polymerization reaction, enlarging the effective surface area of the sensor. The nano gold doping also facilitated charge transfer when exposed to redox reagents. It enabled efficient blocking of the charge transfer upon the occupation of the cavities by cortisol, resulting in enhanced detection response and sensitivity. The Au@MIP sensor exhibited a high affinity toward cortisol binding with a dissociation constant K-d of similar to 0.47 nM, a linear detection range from 1 pM to 500 nM with a detection limit of similar to 200 fM, and satisfied specificity over other steroid hormones with highly similar structures. The sensor was successfully demonstrated to determine cortisol levels in spiked saliva in normal and elevated ranges. The facile antibody-free cortisol detection method was proved to be highly sensitive and selective, suitable for point-of-care testing applications.

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