Sai Bi

An ionic liquid-modified graphene based molecular imprinting electrochemical sensor for sensitive detection of bovine hemoglobin.

A novel kind of molecular imprinted polymers based on ionic liquid-functionalized graphene (MIPs/IL/GR) was prepared by electro-polymerization, which was applied as a molecular recognition element to modify glassy carbon electrode (GCE) to construct an electrochemical sensor (MIPs/IL/GR/GCE) for sensitive detection of bovine hemoglobin (BHb). The fabrication conditions that affect the performance of the imprinted sensor, such as pyrrole concentration, scan cycles and scan rates, have been discussed. Under the optimized conditions, the prepared molecular imprinting electrochemical sensor showed a fast rebinding dynamics, which was successfully applied to BHb detection with a wide linear range from 1.0 × 10(-10) to 1.0 × 10(-3)g/L (R=0.998) and a detection limit of 3.09 × 10(-11)g/L. Moreover, the fabricated sensor possessed a good selectivity and stability, providing a promising tool for immunoassays and clinical applications.

Target-Catalyzed DNA Four-Way Junctions for CRET Imaging of MicroRNA, Concatenated Logic Operations, and Self-Assembly of DNA Nanohydrogels for Targeted Drug Delivery

Here we report a target-catalyzed DNA four-way junction (DNA-4WJ) on the basis of toehold-mediated DNA strand displacement reaction (TM-SDR), which is readily applied in enzyme-free amplified chemiluminescence resonance energy transfer (CRET) imaging of microRNA. In this system, the introduction of target microRNA-let-7a (miR-let-7a) activates a cascade of assembly steps with four DNA hairpins, followed by a disassembly step in which the target microRNA is displaced and released from DNA-4WJ to catalyze the self-assembly of additional branched junctions. As a result, G-quadruplex subunit sequences and fluorophore fluorescein amidite (FAM) are encoded in DNA-4WJ in a close proximity, stimulating a CRET process in the presence of hemin/K(+) to form horseradish peroxidase (HRP)-mimicking DNAzyme that catalyzes the generation of luminol/H2O2 chemiluminescence (CL), which further transfers to FAM. The background signal is easily reduced using magnetic graphene oxide (MGO) to remove unreacted species through magnetic separation, which makes a great contribution to improve the detection sensitivity and achieves a detection limit as low as 6.9 fM microRNA-let-7a (miR-let-7a). In addition, four-input concatenated logic circuits with an automatic reset function have been successfully constructed relying on the architecture of the proposed DNA-4WJ. More importantly, DNA nanohydrogels are self-assembled using DNA-4WJs as building units after centrifugation, which are driven by liquid crystallization and dense packaging of building units. Moreover, the DNA nanohydrogels are readily functionalized by incorporating with aptamers, bioimaging agents, and drug loading sites, which thus are served as efficient nanocarriers for targeted drug delivery and cancer therapy with high loading capacity and excellent biocompatibility.

Initiator-catalyzed self-assembly of duplex-looped DNA hairpin motif based on strand displacement reaction for logic operations and amplified biosensing

Here we program an initiator-catalyzed self-assembly of duplex-looped DNA hairpin motif based on strand displacement reaction. Due to the recycling of initiator and performance in a cascade manner, this system is versatilely extended to logic operations, including the construction of concatenated logic circuits with a feedback function and a biocomputing keypad-lock security system. Compared with previously reported molecular security systems, the prominent feature of our keypad lock is that it can be spontaneously reset and recycled with no need of any external stimulus and human intervention. Moreover, through integrating with an isothermal amplification technique of rolling circle amplification (RCA), this programming catalytic DNA self-assembly strategy readily achieves sensitive and selective biosensing of initiator. Importantly, a magnetic graphene oxide (MGO) is introduced to remarkably reduced background, which plays an important role in enhancing the signal-to-noise ratio and improving the detection sensitivity. Therefore, the proposed sophisticated DNA strand displacement-based methodology with engineering dynamic functions may find broad applications in the construction of programming DNA nanostructures, amplification biosensing platform, and large-scale DNA circuits.

Ag2Te quantum dots with compact surface coatings of multivalent polymers: ambient one-pot aqueous synthesis and the second near-infrared bioimaging.

In this study, we described a facile ambient one-pot aqueous synthesis of fluorescent Ag2Te quantum dots (QDs) adopting multivalent polymers (poly(maleic anhydride) homopolymers) as stabilizers. In experiments, Ag2Te QDs were synthesized via a stepwise addition of the stabilizers, precursors (AgNO3/Na2TeO3) and promoters (NaBH4/N2H4 · H2O) in ambient one-pot aqueous solution. By regulating the compositions of raw materials, water-dispersed Ag2Te QDs (3.8-4.7 nm) were achieved and exhibited tunable photoluminescence (PL) emission (995-1068 nm) in the second near-infrared (NIR-II) region, accompanying with the minimized surface coating thickness (1.5-1.9 nm). Such compact coating of multivalent polymers promoted PL emission of Ag2Te QDs, so showing high PL quantum yields (PLQYs: 13.1-15.2%). In addition to compact sizes and high PLQYs, experimental results testified that the Ag2Te QDs demonstrated high photo-/colloidal stability and ultralow cytotoxicity, which implied their promising applications, especially serving as an effective nanoprobe for bioimaging in the NIR-II biological window.

An electrochemical sensor for the sensitive detection of rutin based on a novel composite of activated silica gel and graphene

In this paper, a novel activated silica gel (ASiG)–graphene (G) composite was initially fabricated via a simple sonication-induced assembly and used as the substrate material to prepare an electrochemical sensor (ASiG/G/GCE) for the sensitive determination of rutin. Morphology and electrochemical properties of the composite were investigated by transmission electron microscopy (TEM), chronocoulometry, electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and differential pulse voltammetry (DPV). Experimental results revealed that the ASiG/G composite induced a remarkable increase of the redox currents of rutin, which could be attributed to the high surface area and excellent electric conductivity of G, as well as the strong accumulation efficiency of ASiG toward rutin. The peak current from DPV is linearly dependent on the rutin concentration in a range of 0.001 to 1.2 μmol L−1 with a detection limit of 3.3 nmol L−1. The ASiG/G/GCE also exhibited good selectivity and acceptable reproducibility. Moreover, the ASiG/G/GCE was successfully applied to the fast determination of rutin in medicine tablets and human plasma with satisfactory recoveries. Therefore, the present work offers a new way to broaden the analytical applications of functionalized graphene in pharmaceutical research.

Linear light-scattering of gold nanostars for versatile biosensing of nucleic acids and proteins using exonuclease III as biocatalyst to signal amplification.

Gold nanomaterials promise a wide range of potential applications in chemical and biological sensing, imaging, and catalysis. In this paper, we demonstrate a facile method for room-temperature synthesis of gold nanostars (AuNSs) with a size of ~50 nm via seeded growth. Significantly, the AuNSs are found to have high light-scattering properties, which are successfully used as labels for sensitive and selective detection of nucleic acids and proteins by using exonuclease III (Exo III) as a biocatalyst. For DNA detection, the binding of targets to the functionalized AuNS probes leads to the Exo III-stimulated cascade recycling amplification. As a result, a large amount of AuNSs are released from magnetic nanoparticles (MNPs) into solution, providing a greatly enhanced light-scattering signal for amplified sensing process. Moreover, a binding-induced DNA three-way junction (DNA TWJ) is introduced to thrombin detection, in which the binding of two aptamers to thrombin triggers assembly of the DNA motifs and initiates the subsequent DNA strand displacement reaction (SDR) and Exo III-assisted cascade recycling amplification. The detection limits of 89 fM and 5.6 pM are achieved for DNA and thrombin, respectively, which are comparable to or even exceed that of the reported isothermal amplification methods. It is noteworthy that based on the DNA TWJ strategy the sequences are independent on target proteins. Additionally, the employment of MNPs in the assays can not only simplify the operations but also improve the detection sensitivity. Therefore, the proposed amplified light-scattering assay with high sensitivity and selectivity, acceptable accuracy, and satisfactory versatility of analytes provides various applications in bioanalysis.

Lable-free quadruple signal amplification strategy for sensitive electrochemical p53 gene biosensing

A versatile label-free quadruple signal amplification biosensing platform for p53 gene (target DNA) detection was proposed. The chitosan-graphene (CS-GR) modified electrode with excellent electron transfer ability could provide a large specific surface for high levels of AuNPs-DNA attachment. The large amount of AuNPs could immobilize more capture probes and enhance the electrochemical signal with the excellent electrocatalytic activity. Furthermore, with the assist of N.BstNB I (the nicking endonuclease), target DNA could be reused and more G-quadruplex-hemin DNAzyme could be formed, allowing significant signal amplification in the presence of H2O2. Such strategy can enhance the oxidation-reduction reaction of adsorbed methylene blue (MB) and efficiently improve the sensitivity of the proposed biosensor. The morphologies of materials and the stepwise biosensor were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM) and cyclic voltammetry (CV). Differential pulse voltammetry (DPV) signals of MB provided quantitative measures of the concentrations of target DNA, with a linear calibration range of 1.0 × 10(-15)-1.0 × 10(-9)M and a detection limit of 3.0 × 10(-16)M. Moreover, the resulting biosensor also exhibited good specificity, acceptable reproducibility and stability, indicating that the present strategy was promising for broad potential application in clinic assay.

A target-initiated DNA network caged on magnetic particles for amplified chemiluminescence resonance energy transfer imaging of microRNA and targeted drug delivery

Chemiluminescence resonance energy transfer (CRET) DNA networks are constructed on magnetic particles initiated by target microRNA, which are further functionalized with aptamers for targeted drug delivery.

Aptamer-functionalized hydrogel as effective anti-cancer drugs delivery agents.

An aptamer-functionalized hydrogel has been developed, which can be regulated by the AS1411 aptamer with the sol-gel conversion. Also the hydrogel can be further utilized for the controlled encapsulation and release of the cancer drugs. Specially, the AS1411 initiates the hybridization of acrydite-modified oligonucleotides to form the hydrogels and the presence of the target protein nucleolin leads the gel to dissolve as a result of reducing the cross-linking density by competitive target-aptamer binding. Based on the rheology of hydrogels, it is possible to utilize this material for storing and releasing molecules. In this research, the cancer drug doxorubicin is encapsulated inside the gel during the formation of the hydrogel and then released in the presence of nucleolin. Further experiments are carried out to prove the specific recognition of target matter. In vitro researches confirm that the aptamer-functionalized hydrogels can be used as drug carriers in targeted therapy and other biotechnological applications.

Cross-catalytic hairpin assembly-based exponential signal amplification for CRET assay with low background noise

A toehold-mediated strand displacement (TMSD)-based cross-catalytic hairpin assembly (C-CHA) is demonstrated in this study, achieving exponential amplification of nucleic acids. Functionally, this system consists of four hairpins (H1, H2, H3 and H4) and one single-stranded initiator (I). Upon the introduction of I, the first CHA reaction (CHA1) is triggered, leading to the self-assembly of hybrid H1·H2 that then initiates the second CHA reaction (CHA2) to obtain the hybrid H3·H4. Since the single-stranded region in H3·H4 is identical to I, a new CHA1 is initiated, which thus achieves cross operation of CHA1 and CHA2 and exponential growth kinetics. Interestingly, because the C-CHA performs in a cascade manner, this system can be considered as multi-level molecular logic circuits with feedback mechanism. Moreover, through incorporating G-quadruplex subunits and fluorescein isothiocyanate (FITC) in the product of H1·H2, this C-CHA is readily utilized to fabricate a chemiluminescence resonance energy transfer (CRET) biosensing platform, achieving sensitive and selective detection of DNA and microRNA in real samples. Since the high background signal induced by FITC in the absence of initiator is greatly reduced through labeling quencher in H1, the signal-to-noise ratio and detection sensitivity are improved significantly. Therefore, our proposed C-CHA protocol holds a great potential for further applications in not only building complex autonomous systems but also the development of biosensing platforms and DNA nanotechnology.