An electrochemiluminescent magneto-immunosensor for ultrasensitive detection of hs-cTnI on a microfluidic chip

Abstract

Sensitive detection and precise quantitation of trace-level crucial biomarkers in a complex sample matrix has become an important area of research. For example, the detection of high-sensitivity cardiac troponin I (hs-cTnI) is strongly recommended in clinical guidelines for early diagnosis of acute myocardial infarction. Based on the use of an electrode modified by single-walled carbon nanotubes (SWCNTs) and a Ru(bpy)32+-doped silica nanoparticle (Ru@SiO2)/tripropylamine (TPA) system, a novel type of electrochemiluminescent (ECL) magneto-immunosensor is developed for ultrasensitive detection of hs-cTnI. In this approach, a large amount of [Ru(bpy)3]2+ is loaded in SiO2 (silica nanoparticles) as luminophores with high luminescent efficiency and SWCNTs as electrode surface modification material with excellent electrooxidation ability for TPA. Subsequently, a hierarchical micropillar array of microstructures is fabricated with a magnet placed at each end to efficiently confine a single layer of immunomagnetic microbeads on the surface of the electrode and enable 7.5-fold signal enhancement. In particular, the use of transparent SWCNTs to modify a transparent ITO electrode provides a two-order-of-magnitude ECL signal amplification. A good linear calibration curve is developed for hs-cTnI concentrations over a wide range from 10 fg/ml to 10 ng/ml, with the limit of detection calculated as 8.720 fg/ml (S/N = 3). This ultrasensitive immunosensor exhibits superior detection performance with remarkable stability, reproducibility, and selectivity. Satisfactory recoveries are obtained in the detection of hs-cTnI in human serum, providing a potential analysis protocol for clinical applications.