Dual-Wavelength Electrochemiluminescence Ratiometry Based on Resonance Energy Transfer between Au Nanoparticles Functionalized g-C₃N₄ Nanosheet and Ru(bpy)₃²⁺ for microRNA Detection

Abstract

Here, a dual-wavelength ratiometric electrochemiluminescence (ECL) approach is reported based on resonance energy transfer (RET) from graphite-like carbon nitride nanosheet (g-C3N4 NS) to Ru­(bpy)3 2+ for sensitive detection of microRNA (miRNA). In this approach, Au nanoparticles (Au NPs) functionalized g-C3N4 NS nanohybrid (Au-g-C3N4 NH) coated on glassy carbon electrode (GCE) could exhibit strong and stable ECL emissions with emission peak centered at 460 nm. The ECL emission at such wavelength matched well with the absorption peak of Ru­(bpy)3 2+ as well as impeccably stimulating the emission of Ru­(bpy)3 2+ at the wavelength of 620 nm, producing ECL-RET with high efficiency. Thus, based on the ECL signals quenching at 460 nm and increasing at 620 nm, a dual-wavelength ratiometric ECL-RET system was achieved. This system was then utilized for determination of target miRNA. With the attachment of thiol-modified molecular beacon on Au-g-C3N4 NH, target miRNA hybridized with the molecular beacon to form a DNA-RNA duplex. The obtained DNA-RNA duplex could be cleaved by duplex-specific nuclease to release target miRNA which would take part in the next cycle for further hybridization. Finally, the introducing of Ru­(bpy)3 2+ was through the probe DNA-Ru­(bpy)3 2+ complementary with the rest single-strand DNA on electrode. By measuring the ratio of ECL460 nm/ECL620 nm, we could accurately quantify the concentration of miRNA-21 in a wide range from 1.0 fM to 1.0 nM. This work provides an important reference for the study of dual-wavelength ECL ratiometry and also exhibits potential capability in the detection of nucleic acids.

Metal/Graphitic Carbon Nitride Composites: Synthesis, Structures, and Applications

“…[139] The conductive polymer PANI improves electrical conductivity in g-C 3 N 4 .U nder optimum conditions, the dopamine concentration increased and the ECL signall inearly increased.T he linear range of dopamined etectionw as 5.0 10 À9 to 1.6 10 À6 m,w ith al ow detection limit of 1.7 10 À6 m.T his sensor exhibited high sensitivity for the detectiono fd opamine. Feng et al reportedt hat g-C 3 N 4 nanohybrid functionalized with gold NPs (Au/g-C 3 N 4 )c ould be used in ad ual-wavelength ratiometric ECL approach for the sensitive detection of microRNA (miRNA), [140] based on resonance energy transfer (RET) from g-C 3 N 4 nanosheets to [Ru(bpy) 3 ] 2 + (bpy = 2,2'-bipyridine). This methodw as more reliable than single-wavelength ECL detection.…”

Recent Advances in Graphitic Carbon Nitride-Based Chemiluminescence, Cataluminescence and Electrochemiluminescence

“…11 Schematic illustration of the dual-wavelength ratiometric ECL-RET biosensor configuration strategy. Reprinted with permission [151] Shang et al proposed a different strategy for dual-signaling-responsive ECL sensor [155], in which the dual-ECL signals could be actuated by different ECL reactions merely from graphite-phase polymeric carbon nitride (GPPCN) nanosheets at anodic and cathodic potentials with triethanolamine and S 2 O 8 2-as co-reactants, respectively. Interestingly, the different metal ions exhibited distinct quenching/enhancement of the ECL signal at different driven potentials, presumably ascribed to the diversity of energy-level matches between the metal ions and GPPCN nanosheets and catalytic interactions of the intermediate species in ECL reactions.…”

Comparison study of electrochemiluminescence of boron-dipyrromethene (BODIPY) dyes in aprotic and aqueous solutions

“…The poor reversibility of the reduction reactions, as seen in the decreased height of the corresponding anodic peak, suggests that the radical anions are less stable than the radical cations. The formal potentials for the first oxidation and reduction peaks were calculated using equation 3 [9], to be -1.305 V and 1.037 V respectively, where E max is the peak potential and ΔE is the pulse height (positive for the anodic scan and negative for the cathodic scan). BODIPY1 is unsubstituted at positions 2 and 6; Bard has demonstrated in the past that BODIPY dyes with such structures tend to exhibit decreased radical cation stability [36].…”

“…Since the 1960s, ECL has expanded to a variety of analytical applications [7], including biological analyses [8][9][10][11][12], cancer biomarker detection [13], and cell surface characterization [14]. In such applications, ECL has advantages over traditional detecting techniques because it does not require a light source [2,5].…”