Abstract
In the last decade, saliva has been suggested as non-invasive diagnostic fluid, suitable for clinical use alternatively to blood serum and plasma. However, the clinical applicability of saliva has been hampered so far by the inadequate sensitivity of current methods to detect the lower salivary concentrations of many biomarkers monitored in blood products. Herein, a label-free biosensor based on electrolyte-gated organic thin-film transistor (EGOTFT) has been developed for the detection at the physical limit of C-reactive protein (CRP) in human saliva. CRP is a key relevant biomarker for inflammatory processes and is routinely monitored for many clinical purposes. Herein, an electrolyte-gated thin-film transistor (EGOTFT) has been proposed as a transducer of the biorecognition event taking place at the gate electrode, functionalized with a self-assembled monolayer (SAM) of highly densely packed capturing anti-CRP proteins. Thanks to the SAM, the biosensing platform herein proposed is endowed with ultra-high sensitivity, along with an extremely high selectivity, assessed by measuring the dose curves of CRP interacting with a bovine serum albumin-functionalized gate. Moreover, the biosensing platform is compatible with low-cost fabrication techniques and applicable to the ultra-sensitive detection of a plethora of clinically relevant biomarkers. Therefore, the EGOTFT device herein proposed, being able to operate in physiologically relevant fluids such as saliva, will set the ground to a major revolution in biosensing applications for early clinical detection.
Highlights
Published in the topical collection Young Investigators in (Bio-)Analytical Chemistry with guest editors Erin Baker, Kerstin Leopold, Francesco Ricci, and Wei Wang.20500 Turku, FinlandThe analysis of human biofluids, such as the blood, urine, saliva, tears, and sweat, yields useful clinical information for the evaluation and monitoring of health and disease states [1]
Among the plethora of biomarkers whose quantification in saliva could potentially contribute to monitor the onset of many pathological states, C-reactive protein (CRP) has attracted a great deal of attention
The SiMoT used in this study is based on an electrolyte-gated organic thin-film transistor (EGOTFT) embedding P3HT as organic semiconductor, which forms a conductive channel between source and drain contacts, and water as electrolyte medium
Summary
Published in the topical collection Young Investigators in (Bio-)Analytical Chemistry with guest editors Erin Baker, Kerstin Leopold, Francesco Ricci, and Wei Wang.20500 Turku, FinlandThe analysis of human biofluids, such as the blood, urine, saliva, tears, and sweat, yields useful clinical information for the evaluation and monitoring of health and disease states [1]. The diffusion of saliva has clinically relevant biofluid has been hindered so far by the insufficient sensitivity of current analytical methods to detect the lower salivary concentrations of many biomarkers compared to blood products [13]. Because of its nonlipophilic structure and high molecular weight, CRP shows limited transfer from the blood to saliva [28] All these call for the development of a label-free ultra-highly sensitive clinical assays [29], capable of tracking a biomarker down to the physical limit and compatible with point-of-care testing. In this perspective, the main barrier is the development of a biosensing platform being able to detect single molecules with a sufficiently large signal to noise ratio [30]. The SiMoT biosensing platform has been engaged in the detection of CRP in a diluted sample of real human saliva, proving that single-molecule detection is possible real samples
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