Shared hairpin structure electrochemiluminescence biosensor based on Au@Ni-Co metal organic frameworks for simultaneous detection of Pb(II) and S.aureus.

The excessive content of lead (Pb(II)) and Staphylococcus aureus (S.aureus) seriously harms the quality of aquatic products. In this paper, a highly sensitive electrochemiluminescence (ECL) biosensor was constructed using the synergistic effect of Au NPs@Nickel-Cobalt-Metal-organic frameworks (Au@Ni-Co-MOFs) and double potential resolution function of urchin-like Au@luminol and Cadmium sulfide quantum dots (CdS QDs) for synchronous detection of Pb(II) and S.aureus in aquatic products. Au@Ni-Co-MOFs as the base material, its cube structure can improve the surface active area and sensitivity of the sensor, providing more catalytic active sites for the two functional probes. Urchin-like Au@luminol binding aptamer DNA2 specifically recognizes Pb(II), CdS QDs binding aptamer DNA3 specifically recognizes S.aureus, which collaboratively catalyzed hydrogen peroxide reduction to produce two electrochemiluminescence signals. The shared hairpin structure DNA1 binds stably to Au@Ni-Co-MOFs via the Au-S bond, and the two functional probes are complementary paired with the DNA1 respectively to ensure the specificity of the aptamer. According to the ECL intensity changes of different potentials signal sources, the synchronous detection of Pb(II) and S.aureus with different concentrations is realized. The sensor realizes the detection of two targets in aquatic products and provides a new strategy for the simultaneous detection of multiple targets.

Bipotential-resolved electrochemiluminescence biosensor based on Bi2S3@Au nanoflowers for simultaneous detection of Cd(II) and ampicillin in aquatic products.

In this paper, an electrochemiluminescence (ECL) biosensor was constructed using Bi2S3@Au nanoflowers as the based nanomaterial and Au@luminol and CdS QDs as independent ECL emission signal respectively. As the substrate of the working electrode, Bi2S3@Au nanoflowers improved the effective area of electrode and accelerated electron transfer rate between gold nanoparticles and aptamer, provided a good interface environment for the loading of luminescent materials. Then, the Au@luminol functionalized DNA2 probe was used as an independent ECL signal source under positive potential and recognized Cd(II), while the CdS QDs functionalized DNA3 probe was used as an independent ECL signal source under negative potential and recognized ampicillin. The simultaneous detection of Cd(II) and ampicillin in different concentrations are realized. This sensor not only has good selectivity and high sensitivity in real sample detection, but also open up a novel way to construct multi-target ECL biosensor for simultaneous detection.

A dual-modal electrochemical aptasensor based on intelligent DNA Walker with cascade signal amplification powered by Nb.BbvCI for Pb2.

As a unique nanomachine, DNA Walker can move continuously along a specific orbit to amplify signal. Therefore, based on DNA Walker and endonuclease assisted signal amplification strategy, a novel dual-mode visual electrochemical aptasensor was constructed for the detection of Pb2+. Ceric dioxide@mesoporous carbon (CeO2/CS)@AuNPs not only could improve the conductivity of sensing interface but also could fix the aptamer. DNA Walker moved on the surface of the electrode to realize the pairing with the Ag-γFe2O3/cDNA probe, forming a special base sequence that could be spliced by the Nb.BbvCI. Under the action of endonuclease Nb.BbvCI, the Ag-γFe2O3/cDNA probe was continuously sheared and the amount on the electrode was decreased to amplify the signal. Besides, the nanoenzyme of Ag-γFe2O3 could catalyze 3'3'5'5'-tetramethylbenzidine (TMB) to blue color realizing the visual detection of Pb2+. The sensor has been successfully applied to the visual and accurate rapid detection of Pb2+ in aquatic products. The fabricated method of the sensor open up a new way for visual and accurate the detection of environmental pollutants.

Dual-target electrochemical DNA sensor for detection of Pb2+ and Hg2+ simultaneously by exonuclease I-assisted recycling signal amplification.

With the development of exonuclease, the exonuclease has been used to construct a variety of aptasensor and to realize the signal amplification. Among them, based on silver nanoparticles (Ag NPs) and exonuclease I (Exo I)-assisted cycle signal amplification strategy, we designed a novel high-sensitivity dual-target electrochemical biosensor to detect Pb2+ or Hg2+ in water. In the presence of Hg2+, the Hg2+ was fixed to the aptamer chain by thymine-Hg2+-thymine (T-Hg2+-T), resulting in the decrease of signal. When Pb2+ was present, DNA single strand S2 dissociated and was bound to Pb2+, which automatically triggered Exo I to selectively cut the single chain from the recognition site to achieve the cyclic amplification of the electrochemical signal. The interaction between aptamer and Exo I was investigated by gel electrophoresis. Under the optimum conditions in the scan range -0.20 to 0.60 V, the biosensor had high sensitivity with a linear range of 100 pg/L to 10.0 mg/L, Pb2+ or Hg2+, and the detection limits were 17.0 pg/L (R2 = 0.993) and 12.0 pg/L (R2 = 0.993), respectively. The relative standard deviation (RSD) of the sensor was 0.5-2.6%, and the recovery of spiked standard solutions was between 98.3 and 110%. The cycle amplification strategy supported by this enzyme has promising applications in detection of the two metal ions in various fields.

Electrochemiluminescence biosensor for determination of lead(II) ions using signal amplification by Au@SiO2 and tripropylamine-endonuclease assisted cycling process.

MXene@Au as the base and Au@SiO2 as signal amplification factor were used for constructing an ultrasensitive "on-off" electrochemiluminescence (ECL) biosensor for the detection of Pb2+ in water. The use of MXene@Au composite provided a good interface environment for the loading of tris(2,2-bipyridyl)ruthenium(II) (Ru(bpy)32+) on the electrode. Based on resonance energy transfer, the Au (core) SiO2 (shell) (Au@SiO2) nanoparticles stimulate electron transport and promote tripropylamine (TPrA) oxidation. The luminescence effect of Au@SiO2 was five times that of AuNPs and SiO2 nanomaterials alone, and the ECL intensity was greatly improved. In addition, Pb2+ activated the aptamer to exert its endonuclease activity, which realized the signal cycle amplification in the process of Pb2+ detection. When Pb2+ was added, the ECL signal weakened, and the Pb2+ concentration was detected according to the decreased ECL intensity. Under optimized experimental conditions, this aptamer sensor for Pb2+ has a wide detection range (0.1 to 1 × 106 ng L-1) and a low detection limit (0.059 ng L-1). The relative standard deviation (RSD) of the sensor is 0.39-0.99%, and the recovery of spiked standard is between 90.00 and 125.70%. The sensor shows good selectivity and high sensitivity in actual water sample analysis. This signal amplification strategy possibly provides a new method for the detection of other heavy metal ions and small molecules.

A novel electrochemiluminescence aptasensor based on copper-gold bimetallic nanoparticles and its applications.

In this work, a novel electrochemiluminescence (ECL) aptasensor was structured for the detection of four organophosphorus pesticides (OPs). Firstly, multi-walled carbon nanotubes (MWCNTs) were used to create a favorable loading interface for the fixation of tris (2, 2'-bipyridyl) ruthenium (II) (Ru (bpy)32+). At the same time, copper (core)-gold (shell) bimetallic nanoparticles (Cu@Au NPs) were synthesized in the aqueous phase for the sensor construction. Gold nanoparticles (Au NPs) could promote the electrochemiluminescence intensity of Ru (bpy)32+ with high efficiency by catalyzing the oxidation process of tri-n-propylamine (TPrA). Compared with the Au NPs, Cu@Au NPs increased the solid loading of Au NPs by virtue of the large specific surface area of copper nanoparticles (Cu NPs), which could further improve the sensitivity of aptasensor. When OPs were added, the ECL intensity was significantly reduced, and the concentration of OPs could be detected through the ECL intensity. Under the optimum conditions, the aptasensor had a wider dynamic range and ultra-low detection limit for the detection of four pesticides: profenofos, isocarbophos, phorate, and omethoate, and their detection limits were 3 × 10-4 ng/mL, 3 × 10-4 ng/mL, 3 × 10-3 ng/mL, and 3 × 10-2 ng/mL respectively (S/N = 3). The aptasensor had the merits of good stability, reproducibility, and specificity, and had a favorable recovery rate in detecting OPs residues in vegetables. This work provided an effective method for the construction of a simple, rapid, and sensitive biosensor.