Quench-Type Electrochemiluminescence Immunosensor Based on Resonance Energy Transfer from Carbon Nanotubes and Au-Nanoparticles-Enhanced g-C₃N₄ to CuO@Polydopamine for Procalcitonin Detection

Abstract

A new type of sandwich electrochemiluminescence (ECL) immunosensor dependent on ECL resonance energy transfer (ECL-RET) to achieve sensitive detection of procalcitonin (PCT) has been designed. In brief, carbon nanotubes (CNT) and Au-nanoparticles-functionalized graphitic carbon nitride (g-C3N4–CNT@Au) and CuO nanospheres covered with polydopamine (PDA) layer (CuO@PDA) were synthesized and applied as ECL donor and receptor, respectively. g-C3N4–CNT nanomaterials were in situ prepared on the basis of π–π conjugation, and the CNT content in the composite were optimized to achieve a strong and stable ECL signal. At the same time, Au nanoparticles were used to functionalize g-C3N4–CNT to further increase the ECL intensity and the loading amount of primary antibody (Ab1). Moreover, CuO@PDA was first used to successfully quench the ECL signal of g-C3N4–CNT@Au. Under the optimum experimental conditions, the linear detection range for PCT concentration was within 0.0001–10 ng mL–1 and the detection limit was 25.7 fg mL–1 (S/N = 3). Considering prominent specificity, reproducibility, and stability, the prepared immunosensor was used to assess recovery rate of PCT in human serum according to the standard addition method and the result was satisfactory. In addition, it is worth mentioning that a novel ECL-RET pair of g-C3N4–CNT@Au (donor)/CuO@PDA (acceptor) was first developed, which offered an effective analytical tool for sensitive detection of biomarkers in early disease diagnostics.

Carbon–Graphitic Carbon Nitride Hybrids for Heterogeneous Photocatalysis

“…On the other hand, the contacted interface of carbon/g‐C 3 N 4 photocatalysts can be automatically positioned by electrochemical surface transfer, where the interfacial potential level acted as donors or acceptors for enhancing gradient photocarrier transportation, thus locally in‐building an electrochemical response to promote electrical conductivity. [ 28,36 ]…”

“…[ 34 ] Specifically, the arranged all‐carbon structure makes carbon materials have variable structure–property relationship through molecular modification and structural engineering. This unique feature endows carbon family present abundant structures, such as 0D carbon dots, [ 33,35 ] 1D carbon nanofibers/nanotubes, [ 36,37 ] 2D graphene nanosheets, [ 38,39 ] and 3D carbon spheres. [ 40 ] The design of carbon‐induced g‐C 3 N 4 photocatalyst not only introduce renewable carbon materials, to further substitute environmentally unfriendly metal‐based materials, but also effectively pave a promising way to sustainable development of photocatalytic technology.…”

Electrochemiluminescence Biosensors Using Screen-Printed Electrodes

“…Considering the different labels attached to secondary antibodies, different configurations of sandwich-type ECL immunosensors have been developed: The traditional sandwich type immunosensor is based on the linkage to the secondary antibody of a luminophore molecule or a nanomaterial, which acts as luminophore itself or is used as support to attach a great number of luminophore molecules. The quench-type electrochemiluminescence immunosensor uses a secondary antibody linked to an element capable of generating resonance energy transfer (RET) phenomena of the emitting specie [ 60 , 61 ]. The element capable of quenching the ECL emission is usually a nanomaterial or a composite nanomaterial, decreasing the ECL emission when higher amounts of analytes are present in the sample.…”

“…The quench-type electrochemiluminescence immunosensor uses a secondary antibody linked to an element capable of generating resonance energy transfer (RET) phenomena of the emitting specie [ 60 , 61 ]. The element capable of quenching the ECL emission is usually a nanomaterial or a composite nanomaterial, decreasing the ECL emission when higher amounts of analytes are present in the sample.…”

Emerging tri‐s‐triazine‐based graphitic carbon nitride: A potential signal‐transducing nanostructured material for sensor applications

“…Adapted and reproduced with permission. [ 17–28 ] Copyright 2019, 2018 and 2017, Elsevier; Copyright 2017, Springer; Copyright 2018, 2015 and 2020 American Chemical Society; Copyright 2017 and 2019, The Royal Society of Chemistry…”