Aggregation-Induced Enhanced Electrochemiluminescence Resonance Energy Transfer Biosensor for Ultrasensitive Detection of Carcinoembryonic Antigen Based on Donor-Acceptor Organic Nanoparticles.

Aggregation-induced electrochemiluminescence (AIECL) combines the merits of aggregation-induced emission (AIE) and electrochemiluminescence (ECL), which has become a research hot spot in recent years. Therefore, we synthesized a novel AIE compound (Z)-3-(4-(2-butyl-1,3-dioxo-2,3-dihydro-1H-benzo[de]isoquinolin-6-yl)phenyl)-2-(4-(1,2,2-triphenylvinyl)phenyl)acrylonitrile (TPENI) with a donor-acceptor (D-A) structure, that is, a simple peripheral modification of 4-(2-butyl-1,3-dioxo-2,3-dihydro-1H-benzo[de]isoquinolin-6-yl) benzaldehyde (NI-CHO) with AIE-active tetraphenylethylene (TPE) to achieve the transition of NI-CHO from aggregation-caused quenching (ACQ) to an AIE molecule. When TPENI was in the aggregated state, the luminescence intensity was significantly enhanced due to the TPE structural unit restricting the free rotation of the intramolecular benzene ring, as well as the π-π stacking interactions of the molecules, which was conducive to the preparation of TPENI NPs as ECL materials. Satisfactorily, we found that the ECL intensity of TPENI NPs was increased by about 4.8-fold compared with that of the molecules dispersed in organic solution, and the stability reached about 1000 s. Based on the excellent ECL properties of TPENI NPs, an "on-off-on" ECL biosensor with a wider detection range (1 fg/mL to 100 ng/mL) and a lower detection limit of 0.20 fg/mL (S/N = 3) was proposed for sensitive analysis of a carcinoembryonic antigen (CEA). Overall, this work provided a new approach to the realization of AIECL and laid the foundation for the application of naphthalimide derivatives in ECL.

A sandwich-type photoelectrochemical biosensor based on Ru(bpy)32+ sensitized In2S3 for aflatoxin B1 detection.

Aflatoxin B1 (AFB1), classified as a class I carcinogen, is a widespread mycotoxin that poses a serious threat to public health and economic development, and the food safety problems caused by AFB1 have aroused worldwide concern. The development of accurate and sensitive methods for the detection of AFB1 is significant for food safety monitoring. In this work, a sandwich-type photoelectrochemical (PEC) biosensor for AFB1 detection was constructed on the basis of an aptamer-antibody structure. A good photocurrent response was obtained due to the sensitization of In2S3 by Ru(bpy)32+. In addition, this sandwich-type sensor constructed by modification with the antibody, target detector, and aptamer layer by layer attenuated the migration hindering effect of photogenerated carriers caused by the double antibody structure. The aptamer and antibody synergistically recognized and captured the target analyte, resulting in more reliable PEC response signals. CdSe@CdS QDs-Apt were modified as a signal-off probe onto the sensor platform to quantitatively detect AFB1 with a "signal-off" response, which enhanced the sensitivity of the sensor. The PEC biosensor showed a linear response range from 10-12 to 10-6 g mL-1 with a detection limit of 0.023 pg mL-1, providing a feasible approach for the quantitative detection of AFB1 in food samples.

An electrochemiluminescence aptasensor based on highly luminescent silver-based MOF and biotin-streptavidin system for mercury ion detection.

In this study, for the first time, a silver-based metal-organic framework (Ag-MOF) was synthesized and used as the electrochemiluminescence (ECL) emitter for building an ECL sensor. After modification with chitosan (CS) and gold nanoparticles (Au NPs), the ECL stability of Ag-MOF was improved. To detect mercury ions, a biosensor was constructed using the mercury ion aptamer and steric effect of streptavidin. First, the capture strand (cDNA) with terminal-modified sulfhydryl group was attached to the electrode surface by the Au-S bond. Then, the mercury-ion aptamer (Apt-Hg) modified with biotin was anchored to the electrode by complementary pairing with cDNA. Streptavidin (SA) could be fixed on the electrode by linking with biotin, thereby reducing the ECL signal. However, in the presence of mercury ions, the aptamer was removed and streptavidin could not be immobilized on the electrode. Hence, the ECL signal of the sensor increased with the concentration of mercury ions, which was linear in the range from 1 µM to 300 fM. The detection limit could reach 66 fM (S/N = 3). The sensor provided a new method for the detection of mercury ions.

Coupled electrochemiluminescent and resonance energy transfer determination of microRNA-141 using functionalized Mxene composite.

The electrochemiluminescence and resonance energy transfer (ECL-RET) method was adopted to detect miRNAs, in which the two-dimensional Ti3C2 Mxenes with high surface area modified with CdS:W nanocrystals (CdS:W NCs) were used as ECL signal emitter. Mxenes with a specific surface area of 5.2755 m2/g carried more emitters and promote ECL intensity. As an energy acceptor, BiOCl nanosheets (BiOCl NSs) have a wide UV-Vis absorption peak in the range 250 nm-700 nm, including the emission band of CdS:W NCs with 520 nm emission wavelength. Hence, BiOCl NSs are covalently bound to hairpin DNA 2 by amide bond to quench the ECL signal of CdS:W NCs. In the presence of miRNA-141, the hairpin DNA 1 modified on the GCE was unfold and then paired with hairpin DNA 2 to release miRNA-141 and quench the signal of the ECL biosensor. Then, the concentration signal of miRNA-141 was amplified by catalytic hairpin assembly. The novel specific biosensor demonstrated a satisfactory linear relationship with miRNA-141 in the range 0.6 pM to 4000 pM; the detection limit was as low as 0.26 pM (3 s/m) under the potential of 0 ~ -1.3 V and showed outstanding RSD of 1.19%. The findings of the present work with high accuracy and sensitivity will be of positive significance for the clinical diagnosis of miRNA in the future work. The construction process of the biosensor and electrochemiluminescence mechanism.

A label-free photoelectrochemical immunosensor for carcinoembryonic antigen detection based on a g-C3N4/CdSe nanocomposite.

Herein, a label-free photoelectrochemical immunosensor based on a g-C3N4/CdSe nanocomposite was established and applied to detect carcinoembryonic antigen (CEA). The prepared nanocomposite materials were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), ultraviolet-visible absorption spectroscopy (UV-vis), X-ray photoelectron spectroscopy (XPS), fourier transform infrared spectrometer (FT-IR) and photoluminescence spectroscopy (PL). The results indicate that g-C3N4/CdSe nanocomposite materials were successfully synthesized. In a typical assembly process, the immunosensor was constructed by modifying a fluorine-doped tin oxide (FTO) electrode with poly dimethyl diallyl ammonium chloride (PDDA), the g-C3N4/CdSe nanocomposite, the anti-carcinoembryonic antigen antibody (Ab) and the blocking agent bovine serum albumin (BSA) successively. In the presence of CEA, the photocurrent signal of the prepared immunosensor decreased significantly. Accordingly, under the optimal conditions, a label-free photoelectrochemical immunosensor was established, and it exhibited excellent selectivity and repeatability for CEA detection. The detection limit was 0.21 ng mL-1, and the range was 10 ng mL-1-100 µg mL-1. Simultaneously, the immunosensor also provides a likely sensing device for detecting other protein targets, which is of great significance for early clinical diagnosis.

Highly sensitive electrochemiluminescence biosensor for VEGF165 detection based on a g-C3N4/PDDA/CdSe nanocomposite.

In this work, an electrochemiluminescence (ECL) biosensor was fabricated for the selective detection of vascular endothelial growth factor (VEGF165). g-C3N4/PDDA/CdSe nanocomposites were used as the ECL substrate. Then, DNA labeled at the 5' end with amino groups (DNA1) was immobilized on the surface of g-C3N4/PDDA/CdSe nanocomposite-modified glassy carbon electrode (GCE) by amido linkage. AuNP-labeled target DNA (Au-DNA2) could hybridize with DNA1 to form a double strand. The ECL of the g-C3N4/PDDA/CdSe nanocomposite was efficiently quenched due to the resonance energy transfer between CdSe QDs and Au NPs. After VEGF165 was recognized and bound by Au-DNA2, the double helix was disrupted, and the energy transfer was broken. In this case, Au-DNA2 was released from the electrode surface, and the ECL intensity recovered to a higher level. Under optimal conditions, this ECL biosensor possesses excellent selectivity, accuracy, and stability for VEGF165 detection in a linear range of 2 pg mL-1 to 2 ng mL-1 with a detection limit of 0.68 pg mL-1. In addition, this assay has been successfully applied to the determination of VEGF165 in serum samples. Graphical abstract Schematic representation of the electrochemiluminescence sensor based on a g-C3N4/PDDA/CdSe nanocomposite, which can be determined in the concentration of vascular endothelial growth factor in serum.

Electrochemiluminescence immunoassay for the prostate-specific antigen by using a CdS/chitosan/g-C3N4 nanocomposite.

An electrochemiluminescence (ECL) biosensor was fabricated for the evaluation of prostate specific antigen (PSA). The sensor was developed by successively modifying glassy carbon electrode (GCE) electrodes with CdS/Chito/g-C3N4 nanocomposites and DNA1 was labeled at the 5' end with thiol. The aptamer DNA was labeled at the 3' end with a quencher ferrocene (Fc) was ligated to DNA1 by the principle of complementary base pairing. In the absence of PSA, the ECL intensity signal is effectively quenches through the energy transfer and photoexcitation electron transfer between CdS/Chito/g-C3N4 emitter and quencher Fc. After incubation with target PSA, the aptamer DNA interacts with PSA and then moved away from the electrode surface together, which will recover the ECL intensity. Under the optimal conditions, the ECL intensity increases linearly with the logarithm of PSA concentration in the range of 1 pg·mL-1 to 100 ng·mL-1, and the detection limit is 0.14 pg·mL-1 (S/N = 3). The biosensor has been successfully applied to the determination of PSA in serum sample. Graphical abstractSchematic representation of the electrochemiluminescence sensor based on a CdS/chitosan/g-C3N4 nanocomposite, which can be applied to the determination of prostate specific antigen in serum.

Photoelectrochemical immunoassay for human interleukin 6 based on the use of perovskite-type LaFeO3 nanoparticles on fluorine-doped tin oxide glass.

A film of perovskite-type LaFeO3 nanoparticles (NPs) was deposited on fluorine-doped tin oxide (FTO) conducting glass via dipping-lifting and calcination. Scanning electron microscopy shows that the NPs are evenly distributed on the surface of the glass. The modified glass was further coated with antibody against human interleukin 6 (IL-6) to result in a photoelectrochemical immunosensor for IL-6. The well-established photoelectrochemical immunoassay has a linear current response in the range of 0.1 pg·mL-1 to 0.1 µg·mL-1 and a detection limit as low as 33 fg·mL-1. Graphical abstract Schematic of a novel photoelectochemical immunoassay for the measurement of IL-6 based on perovskite-type LaFeO3 nanoparticles. The immunoassay had a higher sensitivity and may also be applied to other bioanalysis and environment monitoring.

Strong cathode electroluminescence biosensor based on CeO2 functionalized PCN-222@Ag NPs for sensitive detection of p-Tau-181 protein.

Electrochemiluminescence (ECL) biosensors provide a convenient and high sensitivity method for early disease diagnosis. However, creating luminophore arrays relying on powerful ECL signals remains a daunting task. Porphyrin-centered metal organic frameworks (MOFs) exhibit remarkable potential in ECL sensing applications. In this paper, based on a simple one-pot synthesis method, PCN-222@Ag NPs doped with CeO2 was synthesized to enhance the ECL performance. Due to the strong catalytic ability of CeO2, the ECL signal strength of the new material PCN-222@CeO2@Ag NPs is much higher than that of the PCN-222@Ag NPs and PCN-222. The luminous properties of PCN-222@CeO2@Ag NPs become more intense and stable due to the excellent electronic conductivity of Ag NPs. Based on the fact that CuS@PDA composite can quench the ECL signal of PCN-222@CeO2@Ag NPs, we constructed a novel sandwich ECL immune sensor for the detection of phosphorylated Tau 181 (p-Tau-181) protein. The ECL sensor has a great linear relationship with p-Tau-181 protein concentration, ranging from 1 pg/mL to 100 ng/mL. The detection limit is as low as 0.147 pg/mL. This work provides new ideas for developing sensitive ECL sensors for the p-Tau-181 protein, the marker of Alzheimer's disease.

A ZnIn2S4@ReS2/AgInS2-based photoelectrochemical aptasensor for the ultrasensitive detection of kanamycin.

An ultrasensitive photoelectrochemical (PEC) aptasensor was originally designed by using ZnIn2S4/ReS2 as a photoactive material and AgInS2 as a signal amplifier. The signal amplifier AgInS2 was incubated on the terminal of H-DNA (immobilized on the ZnIn2S4/ReS2/FTO surface), leading to an enhanced photocurrent response. Then, due to the introduction of DNA2, the formation of a double-stranded structure caused AgInS2 to keep away from the electrode surface, and the photocurrent was reduced. In the presence of kanamycin, DNA2 was released from the system due to the competition relationship, and a restored photocurrent response was obtained. The combination of ZnIn2S4/ReS2 and AgInS2 accelerated the electron transfer and enhanced the separation efficiency of photogenerated electron-hole pairs, resulting in an improved performance of the PEC aptasensor, which was capable of accurate and sensitive detection of kanamycin in actual samples.

A photoelectrochemical biosensor based on b-TiO2/CdS:Eu/Ti3C2 heterojunction for the ultrasensitive detection of miRNA-21.

A novel photoelectrochemical (PEC) biosensor based on b-TiO2/CdS:Eu/Ti3C2 heterojunction was developed for ultrasensitive determination of miRNA-21. In this device, the b-TiO2/CdS:Eu/Ti3C2 heterojunction with excellent energy level arrangement effectively facilitated photoelectric conversion efficiency and accelerated the separation of the photogenerated electron hole pairs, which because that the structure of heterojunction overcomes the drawbacks of single material, such as narrow light absorption range, wide band gap, short carrier lifetime, etc., improves light utilization, extends the lifetime of photogenerated electron hole pairs, and promotes electron transfer. Herein, hairpin DNA1 (H1) decorated on the b-TiO2/CdS:Eu/Ti3C2 electrode surface by Cd-S bonds, after H2/miRNA-21 heterduplex was introduced, the strand-displacement reaction (SDR) was triggered between H1 and H2/miRNA-21, accordingly, miRNA-21 was discharged from the H2/miRNA-21 heterduplex, forming the H1/H2 duplex, and the reuse of miRNA-21 was realized. As a signal amplification factor, the signal amplification factor H3-CdSe was hybridized with H1/H2 duplex, which greatly enhanced the sensitivity of the PEC biosensor. Under optimal conditions, the designed PEC biosensor displayed outstanding sensitivity, selectivity and stability with a wide liner range from 1.0 µM to 10.0 fM and a low detection limit of 3.3 fM. The preparation of the optoelectronic material affords a new direction for the progress of heterojunction photovoltaic materials and the construction of the proposed biosensor also provides a new thought for the PEC detection of human miRNA-21 with superior performance. Simultaneously, the established biosensor exhibiting tremendous possibility for detecting other biomarkers and biomolecules in clinical diagnosis fields.

ORAOV 1 Detection Made with Metal Organic Frameworks Based on Ti3C2Tx MXene.

In this work, a two-dimensional (2D) MOF sheet with electrochemiluminescence (ECL) activity is prepared with Ti3C2Tx MXene as the metal precursor and the meso-tetra(4-carboxyl-phenyl) porphyrin (H2TCPP) as the organic ligand. The atomically thin 2D Ti3C2Tx MXene is utilized as the metal precursor and soft template to produce the MOF with a 2D nanosheet morphology (Ti3C2Tx-PMOF). Ti3C2Tx MXene is a kind of strong electron acceptor, which can deprotonate H2TCPP due to the high electronegativity and low work function of its terminal atoms. The deprotonated H2TCPP continues to bind with Ti atoms to form the 2D MOF sheet. The ECL activity is inherited from H2TCPP and stabilized by introducing Ag NPs. Then, we construct an ECL biosensor based on the Ag NPs/Ti3C2Tx-PMOF to detect the oral cancer overexpressed 1 (ORAOV 1). A bipedal three-dimensional DNA walker strategy is adopted to further improve the biosensor sensitivity. As expected, the biosensor exhibits sterling sensitivity and selectivity. The ECL biosensor responds linearly to ORAOV 1 concentrations in the range of 10 fM-1 nM, and the detection limit is as low as 3.3 fM (S/N = 3). It means that Ag NPs/Ti3C2Tx-PMOF is a potential material to design and construct the high-performance ECL biosensors.

Electrochemiluminescence aptasensor for lincomycin antigen detection by using a SnO2/chitosan/g-C3N4 nanocomposite.

In this paper, hydrothermal method was used for the synthesis of SnO2 quantum dots (QDs). The prepared SnO2 QDs have a uniform particle size distribution and good electrochemiluminescence (ECL) property. Then the prepared SnO2 QDs was combined with graphene-like carbon nitride (g-C3N4) through chitosan to form SnO2/chitosan/g-C3N4 nanocomposite and used for detecting the lincomycin. The characteristics of SnO2/chitosan/g-C3N4 nanocomposite were presented by transmission electron microscopy (TEM), X-ray diffraction (XRD) and energy dispersive spectroscopy (EDS), and the analytical results proving that the nanocomposite was prepared successfully. In this strategy, the SnO2/chitosan/g-C3N4 nanocomposite was acted as the substrate of aptasensor. Then, SH-DNA (aptamer DNA) was assembled on the surface of electrode, after 6-mercaptohexanol (MCH) blocked the unbound sites of the electrode surface, ferrocene-DNA (Fc-DNA) was incubated on the electrode surface through base complementation with aptamer DNA. In the absence of lincomycin, due to the low conductivity of Fc-DNA and the photo-excited energy electron transfer, the ECL signal was quenched. In the presence of lincomycin, the aptamer DNA was specific binding with lincomycin, and ferrocene-DNA (Fc-DNA) was detached from the surface of aptasensor electrode, generating an obviously enhancement of ECL signal. To ensure the accuracy of the data, each electrode runs continuously for 3600 s. Under optimal experimental conditions, the detection range of the aptasensor was 0.10 ng mL-1 - 0.10 mg mL-1, and the detection limit was 0.028 ng mL-1. In addition, the aptasensor has good stability and reproducibility, and also provided a hopeful device for all kinds of other protein target.

Highly sensitive photoelectrochemical biosensor for microRNA159c detection based on a Ti3C2:CdS nanocomposite of breast cancer.

Herein, an ultra-sensitive photoelectrochemical biosensor based on Ti3C2:CdS nanocomposite was established for the selective detection of microRNA159c. Ti3C2:CdS nanocomposites were used as optoelectronic materials because Ti3C2:CdS interaction effectively separates photogenerated electrons and holes, and significantly improves the high photoelectric conversion efficiency. Firstly, Ti3C2:CdS nanocomposite was deposited on the surface of the fluorine-doped tin oxide (FTO) electrode. After the chitosan (CS) was dropped, the SH-miRNA were bonded on the electrode surface via the S-Cd bond. Then 6-mercaptohexanol (MCH) blocked the unbound site, the DNA strand was introduced to hybridize with the target SH-miRNA. At this time, the obtained photocurrent gradually decreases. Subsequently, the photosensitizer TMPyP as signal amplification was modified, the photocurrent increased significantly. The target SH-miRNA was detected based upon the photocurrent change originated from quantities change of TMPyP. Working under the best experimental conditions, the sensing platform had good stability, selectivity, and high sensitivity. The detection range for miRNA159c was 1.0 × 10-6-1.0 × 10-13 mol·L-l, and the detection limit was approximately 33 fmol·L-l. The detection of miRNA159c in human serum provided a huge opportunity to explore the relationship between the abundance of this miRNA and the incidence of breast cancer (BC), and to further achieve effective detection of BC.

Photoelectrochemical DNA biosensor based on g-C3N4/MoS2 2D/2D heterojunction electrode matrix and co-sensitization amplification with CdSe QDs for the sensitive detection of ssDNA.

A novel enhanced photoelectrochemical (PEC) DNA biosensor, based on a compact heterojunction g-C3N4/MoS2 and co-sensitization effect with CdSe quantum dots (QDs), was first proposed for simple and accurate analysis of a short ssDNA. In this work, the g-C3N4/MoS2 was successfully synthesized and used as the electrode matrix material to construct PEC biosensor. 2D/2D heterojunction was formed between g-C3N4 and MoS2, which could promote the separation of photogenerated electron-hole pairs resulting in an enhanced photocurrent. In the presence of target DNA, CdSe QDs labeled reporter DNA was complementary pairing with target DNA which was specific recognized by capture DNA loading on self-assembled CdS QDs film, leading to close contact between CdSe QDs and g-C3N4/MoS2 modified electrode surface, thereby resulting in the enhanced photocurrent intensity due to the co-sensitization effect. Under the optimal operating conditions, the photoelectrochemical biosensor demonstrated favorable accuracy and could respond to 0.32 pM (S/N = 3) with a linear concentration range from 1.0 pM to 2.0 µM. Moreover, the proposed PEC DNA biosensor exhibits high sensitivity, excellent specificity, acceptable reproducibility and accuracy, showing a promising potential in DNA bioanalysis and other relative fields.

A label-free photoelectrochemical biosensor for urokinase-type plasminogen activator detection based on a g-C3N4/CdS nanocomposite.

Herein, we established a novel ultrasensitive photoelectrochemical biosensor for detecting urokinase-type plasminogen activator (u-PA), based on a g-C3N4/CdS nanocomposite. The prepared nanocomposite was characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, ultraviolet-visible absorption spectroscopy, and Fourier transform infrared spectroscopy, thus indicating that the nanocomposite was prepared successfully. In the typical process, the prepared nanocomposite was deposited on the surface of a bare FTO electrode. After being air-dried, the g-C3N4/CdS nanocomposite modified electrode was successively incubated with antibody against urokinase-type plasminogen activator and the blocking agent BSA to produce a photoelectrochemical biosensor for u-PA. In the presence of target u-PA antigen, the photocurrent response of the prepared biosensor electrode decreased significantly. The proposed novel photoelectrochemical biosensor exhibited good sensitivity, specificity, and reproducibility for u-PA detection, and a low detection limit of 33 fg mL-1, ranging from 1 µg mL-1-0.1 pg mL-1. The proposed strategy should provide a promising method for detection of other biomarkers.

Highly sensitive electrochemical biosensor for streptavidin detection based on CdSe quantum dots.

An electrochemical biosensor was developed based on a steric hindrance hybridization assay to allow the highly sensitive detection of streptavidin. In the steric hindrance hybridization assay, the signaling strand DNA (sig-DNA) was labeled at the 3' end with CdSe quantum dots (QDs) and at the 5' end with biotin, and capturing strand DNA (the complementary strand of sig-DNA) was labeled at the 5' end with thiol. The steric hindrance effect generated by streptavidin which was bound with the signaling DNA strand. The streptavidin limited the ability of the sig-DNA to hybridize with the cap-DNA, which were linked on the surface of a gold electrode. Therefore, the concentration of streptavidin was detected indirectly based on the concentration of CdSe QDs on the electrode surface. The concentration of CdSe QDs on the electrode surface was detected by differential pulse anodic stripping voltammetry. Under optimal conditions, the streptavidin detection range using the as-prepared biosensor was 1.96pg/mL to 1.96µg/mL and the detection limit was 0.65pg/mL. The experimental results showed that the electrochemical biosensor could detect streptavidin rapidly and accurately.

Enhanced photoelectrochemical DNA sensor based on TiO2/Au hybrid structure.

A novel enhanced photoelectrochemical DNA sensor, based on a TiO2/Au hybrid electrode structure, was developed to detect target DNA. The sensor was developed by successively modifying fluorine-tin oxide (FTO) electrodes with TiO2 nanoparticles, gold (Au) nanoparticles, hairpin DNA (DNA1), and CdSe-COOH quantum dots (QDs), which acted as signal amplification factors. In the absence of target DNA, the incubated DNA1 hairpin and the CdSe-COOH QDs were in close contact with the TiO2/Au electrode surface, leading to an enhanced photocurrent intensity due to the sensitization effect. After incubation of the modified electrode with the target DNA, the hairpin DNA changed into a double helix structure, and the CdSe QDs moved away from the TiO2/Au electrode surface, leading to a decreased sensitization effect and photoelectrochemical signal intensity. This novel DNA sensor exhibited stable, sensitive and reproducible detection of DNA from 0.1 µM to 10 fM, with a lower detection limit of 3 fM. It provided good specificity, reproducibility, stability and is a promising strategy for the detection of a variety of other DNA targets, for early clinical diagnosis of various diseases.

A novel electrochemiluminescence biosensor for the detection of microRNAs based on a DNA functionalized nitrogen doped carbon quantum dots as signal enhancers.

An ultrasensitive electrochemiluminescence (ECL) biosensor for the detection of microRNA was developed based on nicking enzymes Nb.BbvCI mediated signal amplification (NESA). First, the hairpin probe1-N-CQDs with assistant probe and microRNA (miRNA) formed Y junction structure which was cleaved with the addition of nicking enzymes Nb.BbvCI to release miRNA and assistant probe. Subsequently, the released miRNA and assistant probe can initiate the next recycling process. The generation of numerous intermediate sequences nitrogen doped carbon quantum dots-DNA (N-CQDs-DNA) can further hybridize with hairpin probe2 immobilized on GO/Au composite modified electrode surface, the initial ECL intensity was enhanced. The ECL intensity would increase with increasing concentration of the target miRNA, and the sensitivity of biosensor would be promoted because of the efficient signal amplification of the target induced cycling reaction. The novel designed biosensor provided a highly sensitive and selective detection of miRNA-21 from 10 aM to104 fM with a relatively low detection limit of 10 aM. Thus, our strategy has a potential application in the clinical diagnosis.

Electrochemical biosensor for Ni(2+) detection based on a DNAzyme-CdSe nanocomposite.

The detection and speciation analysis of metal-ion is very important for environmental monitoring. A novel electrochemical biosensor for Nickel(II) detection based on a DNAzyme-CdSe nanocomposite was developed. We firstly hybridized with capture probe (DNA1) and sequentially with DNA (DNA2) on the gold electrode. Then CdSe QDs were incorporated the specific recognition of DNA2 by covalent assembling. Upon addition of nickel ion into the above system, the substrate strand of the immobilized DNAzyme was catalytically cleaved by target Ni(2+), resulting in disassociation of the shorter DNA fragments containing CdSe QDs. The remaining CdSe QDs on the electrode surface detected by differential pulse anodic stripping voltammetry (DPASV). Under optimal conditions, the as-prepared sensor exhibited high sensitivity and fast response to Ni(2+) with the linear range from 20 nM to 0.2mM and a low detection limit of 6.67 nM. The prepared biosensor also shows good stability and good reproducibility and high selectivity toward target Ni(2+) against other metal ions because of highly specific Ni(2+)-dependent DNAzyme. Thus, our strategy has a good potential in the environment surveys.