Highly Efficient Wavelength-Resolved Electrochemiluminescence of Carbon Nitride Films for Ultrasensitive Multiplex MicroRNA Detection

Abstract

The development of electrochemiluminescence (ECL) emitters of different colors with high ECL efficiency (ΦECL) is appealing yet challenging for ultrasensitive multiplexed bioassays. Herein, we report the synthesis of highly efficient polymeric carbon nitride (CN) films with fine-tuned ECL emission from blue to green (410, 450, 470, and 525 nm) using the precursor crystallization method. More importantly, naked eye-observable and significantly enhanced ECL emission was achieved, and the cathodic ΦECL values were ca. 112, 394, 353, and 251 times those of the aqueous Ru­(bpy)3Cl2/K2S2O8 reference. Mechanism studies showed that the density of surface-trapped electrons, the associated nonradiative decay pathways, and electron–hole recombination kinetics were crucial factors for the high ΦECL of CN. Based on high ΦECL and different colors of ECL emission, the wavelength-resolved multiplexing ECL biosensor was constructed to simultaneously detect miRNA-21 and miRNA-141 with superior low detection limits of 0.13 fM and 25.17 aM, respectively. This work provides a facile method to synthesize wavelength-resolved ECL emitters based on metal-free CN polymers with high ΦECL for multiplexed bioassays.

A novel PEC and ECL bifunctional aptasensor based on V2CTx MXene-derived MOF embedded with silver nanoparticles for selectively aptasensing miRNA-126

“…14 Generally, the sensing principle of ECL sensor is based on the detection interaction between biological recognition elements and corresponding targets via emission intensity change of luminophores. 15,16 In addition, PEC biosensors have demonstrated the advantages of simple instrumentation, ultrahigh detection sensitivity, superior stability, and low background noise, also showing promising application for the analysis of trace miRNAs. 17 The detection mechanism of a PEC sensor is based on the photoelectric chemical effect, which refers to the photosensitive material excited under light stimulation, generating carriers and charge separation and transfer.…”

Electrochemiluminescence resonance energy transfer immunoassay based on a porphyrin metal–organic framework and AuNPs/NSG for the sensitive detection of zearalenone

“…In the field of electrochemiluminescence biosensing, the development of efficient and stable novel ECL luminophores has been the focus of research. 9,11,12 Metal–organic frameworks (MOFs), as emerging molecular crystal materials, have various advantages, such as a large specific surface area, excellent chemical stability and adjustable pore size. 13–15 A variety of MOFs play a key role in electrochemiluminescence biosensing as ECL luminophores.…”

Detection of specific antibodies against SARS-CoV-2 spike protein via ultra-sensitive bio-functionalized carbonnitride-reduced graphene oxide electrochemical immunosensing platform in real samples

“…Simultaneous detection of miRNA-21 and miRNA-141 was carried out using a multiplexed ECL biosensor. 36 Furthermore, mercury monitoring has been reported in water using C 3 N 4 nanosheets. 37 Recently, a photoelectrochemical genosensor has been reported for the detection of SARS-CoV-2 using C 3 N 4 and Au nanoparticles.…”