Chemiluminescence Resonance Energy Transfer-Based Mesoporous Silica Nanosensors for the Detection of miRNA

Abstract

The chemiluminescence resonance energy transfer (CRET)-based method is free of autofluorescence interference, which can achieve an extremely high signal-to-background ratio for detection. Nevertheless, this method is still hindered by the inner filter effect, quenching effect, and nonspecific absorption of reported nanoparticles. Herein, mesoporous silica nanomaterials (MSNs) acted as carriers to load both the donor (horseradish peroxidase, HRP) and the acceptor (a functional DNA duplex). This approach realized the construction of a new CRET-based nanosensor for the sensitive detection of miRNA. By controlling the energy-transfer distance with the designed DNAs, the donor emission at 430 nm could be quenched by the adsorption of the dye labeled on the acceptor DNA. The CRET system could be destroyed by releasing acceptor DNA from linker DNA via the competitive hybridization of target miRNA, resulting in emission recovery for quantification. With the cancer biomarker miR-155 as the model, the sensitive and selective detection of miR-155 was achieved, which showed high energy-transfer efficiency, good specificity, favorable biodegradability, and low toxicity. This work provides a potential pathway for biological detection and clinical diagnosis.

Chemiluminescence Resonance Energy Transfer Efficiency and Donor–Acceptor Distance: from Qualitative to Quantitative

“…As shown in Figure 2 d, the CL spectrum of luminol was recorded in the presence of 5 mM of H 2 O 2 and 10 μM of Co 2+ , which could overlap with the absorption spectra of the micelle solutions of C 8 ‐TPE‐C 4 TAB, C 4 ‐TPE‐C 8 TAB, and TPE‐C 12 TAB [2, 16] . It was worth noting that high CRET efficiency can still be obtained by shortening the donor–acceptor distance in the presence of the small overlap between the emission of donor and the absorption of acceptor [27–29] . Therefore, C 8 ‐TPE‐C 4 TAB, C 4 ‐TPE‐C 8 TAB, and TPE‐C 12 TAB could act as the high‐performance CRET acceptors in the micelles.…”

“…The fluorescence quantum yields of the three micelle solutions (80 μM) were 8.45 %, 15.19 %, and 9.10 %, indicating that the TPE groups could intensely emit in the micelles. In addition, the spectral overlap between donor emission and acceptor absorption was essential for RET to occur [27–29] . As shown in Figure 2 d, the CL spectrum of luminol was recorded in the presence of 5 mM of H 2 O 2 and 10 μM of Co 2+ , which could overlap with the absorption spectra of the micelle solutions of C 8 ‐TPE‐C 4 TAB, C 4 ‐TPE‐C 8 TAB, and TPE‐C 12 TAB [2, 16] .…”

“…[22,24] Thef luorescence quantum yields of the three micelle solutions (80 mM) were 8.45 %, 15.19 %, and 9.10 %, indicating that the TPE groups could intensely emit in the micelles.I na ddition, the spectral overlap between donor emission and acceptor absorption was essential for RET to occur. [27][28][29] As shown in Figure 2d,t he CL spectrum of luminol was recorded in the presence of 5mMo fH 2 O 2 and 10 mMo fC o 2+ ,w hich could overlap with the absorption spectra of the micelle solutions of C 8 -TPE-C 4 TAB, C 4 -TPE-C 8 TAB, and TPE-C 12 TAB. [2,16] It was worth noting that high CRET efficiencyc an still be obtained by shortening the donor-acceptor distance in the presence of the small overlap between the emission of donor and the absorption of acceptor.…”

“…[2,16] It was worth noting that high CRET efficiencyc an still be obtained by shortening the donor-acceptor distance in the presence of the small overlap between the emission of donor and the absorption of acceptor. [27][28][29] Therefore,C 8 -TPE-C 4 TAB, C 4 -TPE-C 8 TAB, and TPE-C 12 TABc ould act as the high-performance CRET acceptors in the micelles.…”

Disordered Assembly of Donors and Acceptors on Layered Double Hydroxides for High-Efficiency Chemiluminescence Resonance Energy Transfer

“…Chemiluminescence (CL) resonance energy transfer (CRET) allows the energy transfer from CL donors to suitable acceptors with high-efficiency luminescence. − CRET has become an attractive candidate for a variety of analytical applications, such as immunoassays, macromolecular analysis, small-molecule detection, and in vitro and in vivo imaging. − To establish an efficient CRET system, two primary considerations must be addressed: (1) minimizing the distance between CL donors and acceptors and (2) maximizing the luminescence efficiency of acceptors. Currently, it is the most convenient approach to bring CL donors and acceptors closer by assembling them into a kind of confined supporter. − However, the closer donor–acceptor distance would usually decrease luminescence efficiency as a result of intrinsic aggregation-caused quenching (ACQ) of acceptors. − Therefore, a versatile strategy is highly required to find a balance between the minimized donor–acceptor distance and high-efficiency luminescence of acceptors.…”