Yueyun Li

A novel label-free electrochemical immunosensor based on functionalized nitrogen-doped graphene quantum dots for carcinoembryonic antigen detection

A novel and ultrasensitive label-free electrochemical immunosensor was fabricated for quantitative detection of carcino-embryonic antigen (CEA). The nitrogen-doped graphene quantum dots (N-GQDs) supported PtPd bimetallic nanoparticles (PtPd/N-GQDs) were synthesized by a simple and green hydrothermal procedure. Subsequently, PtPd/N-GQDs functionalized Au nanoparticles (PtPd/N-GQDs@Au) were prepared successfully via a self-assembly approach. Because of the synergetic effect present in PtPd/N-GQDs@Au, this novel nanocomposites has shown excellent electrocatalytic activity towards hydrogen peroxide (H2O2) reduction. Featuring good biocompatibility, excellent conductivity and large surface area, PtPd/N-GQDs@Au was applied as transducing materials to efficiently conjugate capture antibodies and amplify electrochemical signal. Under the optimal conditions, the proposed immunosensor was used for the detection of CEA with wide dynamic range in the range from 5 fg/mL to 50ng/mL with a low detection limit of 2fg/mL (S/N=3). Furthermore, this label-free immunosensor possesses high sensitivity, special selectivity and long-term stability, which shows promising application in bioassay analysis.

Ultrasensitive non-enzymatic immunosensor for carcino-embryonic antigen based on palladium hybrid vanadium pentoxide/multiwalled carbon nanotubes

A novel and sensitive sandwich-type non-enzymatic electrochemical immunosensor was fabricated for quantitative monitoring of carcino-embryonic antigen (CEA). Nanocomposite of stannic oxide/reduced graphene oxide was used as substrate material to increase the specific surface area and enhance the conductivity of the glassy carbon electrode. Gold nanoparticles (Au NPs) were introduced to link substrate materials and primary antibodies (Ab1) and accelerate the electron transfer in this system. At the same time, the palladium nanoparticles (Pd NPs)-vanadium pentoxide (V2O5)/multiwalled carbon nanotubes (MWCNTs) were used as the label of secondary antibodies (Ab2). This composite label has shown excellent catalytic activity towards the reduction of H2O2. The nanomaterial-based signal amplification can improve the sensitivity and lower the limit of detection. The proposed immunosensor showed wide linear range from 0.5 pgmL(-1) to 25 ngmL(-1) with limit of detection of 0.17 pgmL(-1). This novel immunosensor was used to analyze serum sample. The results indicated that this immunosensor may find huge potential application for quantitative detection of CEA in the clinical diagnosis.

An ultrasensitive sandwich-type electrochemical immunosensor based on the signal amplification strategy of mesoporous core–shell Pd@Pt nanoparticles/amino group functionalized graphene nanocomposite

Herein, a novel and sensitive sandwich-type electrochemical immunosensor was fabricated for quantitative monitoring of prostate specific antigen (PSA). The sulfo group functionalized multi-walled carbon nanotubes (MWCNTs-SO3H) were used as substrate material to increase the specific surface area and enhance the conductivity of the glassy carbon electrode. Gold nanoparticles (Au NPs) were introduced to enhance the load capacity of the substrate material for primary antibodies (Ab1) and accelerate the electron transfer on the electrode interface. The mesoporous core-shell Pd@Pt nanoparticle loaded by amino group functionalized graphene (M-Pd@Pt/NH2-GS) with high specific surface area, high indexed facets, and good biocompatibility was not only as the carriers of secondary antibodies (Ab2) but also catalyzed the reduction of hydrogen peroxide (H2O2), which effectually amplified the current signal in detection of PSA. The as-proposed immunosensor exhibited high sensitivity and stability on the detection of PSA. A linear relationship between current signals and the concentrations of PSA was obtained in the range from 10fg/mL to 50ng/mL and the detection limit of PSA was 3.3fg/mL (signal-to-noise ratio of 3). Furthermore, the as-proposed immunosensor showed excellent performance in detection of human serum samples. The results suggest that the proposed immunosensor will be promising in the diagnostics application for accurately quantitative detection of PSA.

Visible-light driven label-free photoelectrochemical immunosensor based on TiO2/S-BiVO4@Ag2S nanocomposites for sensitive detection OTA

A label-free photoelectrochemical (PEC) platform with high visible-light activity for quantitative detection of the ochratoxin A (OTA) was developed by assembly of Ag2S nanoparticles (NPs) sensitized on titanium dioxide/red blood cell-like shape bismuth vanadate (TiO2/S-BiVO4) electrode via layer-by-layer (LBL) strategy. In this protocol, ascorbic acid was used as an efficient electron donor for scavenging photo-generated holes and inhibiting light driven electron-hole pair recombination. TiO2 has good photoelectric activity and large surface area. The S-BiVO4 with porous structure surfaces can contribute to the high photocurrent intensity under visible-light irradiation. Moreover, the Ag2S NPs were in-situ growth on surfaces of thioglycolic acid modified S-BiVO4, which enhanced photocurrent response and further improved the photocurrent conversion efficiency. Under optimal conditions, the PEC immunosensor exhibited a wide linear concentration range from 5pgmL-1 to 750ngmL-1, with a low detection limit of 1.7pgmL-1 (S/N = 3) for OTA. Additionally, the designed immunosensor was performed with good stability, reproducibility and selectivity, thus opening up a new promising PEC platform for some other small molecules analysis.

A novel sandwich-type electrochemical immunosensor for PSA detection based on PtCu bimetallic hybrid (2D/2D) rGO/g-C3N4.

In this work, a sensitive sandwich-type electrochemical immunosensor was designed for the quantitative detection of prostate-specific antigen (PSA) by amperometric i-t. The Au loaded on thionine functionalized graphene oxide (Au@Th/GO) was used as a platform to immobilize primary antibodies (Ab1) and accelerate the electron transfer on the electrode interface. PtCu bimetallic hybrid were loaded on 2D/2D reduced graphene oxide/graphitic carbon nitride (PtCu@rGO/g-C3N4) with large surface area and biocompatibility, which were employed as labels for combining secondary antibodies (Ab2) and amplifying signals to improve the sensitivity of the designed immunosensor which attributes to its good activity for the reduction of hydrogen peroxide (H2O2). Under optimal conditions, the designed immunosensor exhibited a linear concentration range from 50fg/mL to 40ng/mL, with a low detection limit of 16.6fg/mL (S/N=3) for PSA. Additionally, the designed immunosensor showed acceptable selectivity, reproducibility and stability. The satisfactory results in analyze human serum samples indicated potential application promising in clinical monitoring of tumor markers.

Palladium-Catalyzed 6-Endo Selective Alkyl-Heck Reactions: Access to 5-Phenyl-1,2,3,6-tetrahydropyridine Derivatives.

A new type of palladium-catalyzed 6-endo-selective alkyl-Heck reaction of unactivated alkyl iodides has been described. This strategy provides efficient access to a variety of 5-phenyl-1,2,3,6-tetrahydropyridine derivatives, which are important structural motifs for bioactive molecules. This process displays a broad substrate scope with excellent 6-endo selectivity. Mechanistic investigations reveal that this alkyl-Heck reaction performs via a hybrid palladium-radical process.

An ultrasensitive sandwich-type electrochemical immunosensor based on the signal amplification strategy of echinoidea-shaped Au@Ag-Cu2O nanoparticles for prostate specific antigen detection

Highly sensitive determination of tumor markers plays an important role in early diagnosis of cancer. Herein, a novel and ultrasensitive sandwich-type electrochemical immunosensor was fabricated for quantitative detection of prostate specific antigen (PSA). In this process, gold nanoparticles functionalized nitrogen-doped graphene quantum dots (Au@N-GQDs) was synthesized through a simple and green hydrothermal procedure to enhance conductivity, specific electrode surface area and quantity of immobilized primary antibodies (Ab1). Subsequently, the prepared echinoidea-shaped nanocomposites (Au@Ag-Cu2O) composed of Au@Ag core-shell nanoparticles and disordered cuprous oxide were prepared successfully to label the secondary antibodies (Ab2), which convened the advantages of good biocompatibility and high specific surface area. Because of the synergetic effect present in Au, Ag and Cu2O, the novel nanocomposites exhibited excellent electrocatalytic activity towards the reduction of hydrogen peroxide (H2O2) for the amplified detection of PSA. Therefore, the as-proposed immunosensor for the detection of PSA possessed wide dynamic range from 0.01pg/mL to 100ng/mL with a low detection limit of 0.003pg/mL (S/N = 3). Furthermore, this sandwich-type immunosensor revealed high sensitivity, high selectivity and long-term stability, which had promising application in bioassay analysis.

An optionality further amplification of an sandwich-type electrochemical immunosensor based on biotin–streptavidin–biotin strategy for detection of alpha fetoprotein

An optionality further amplification of sandwich-type electrochemical immunosensor based on Au NPs as platform and biotin-functionalized amination magnetic nanoparticle composite (B-APTES@Fe3O4) as label was designed for detection of alpha fetoprotein (AFP) in this work. The cross-shaped SA has one free biotin-binding site available for carrying a B-Ab2, and the other three binding sites are conjugated with a 3 equimolar ratio of B-APTES@Fe3O4. Thus, further signal amplification could be achieved as SA and B-APTES@Fe3O4 are added layer by layer on the electrode successively. Of the active biotins that were modified on the surface of APTES@Fe3O4, a part of biotins are bound to the SA and the remaining biotins can be used for further connection, which can present a dendritic spread outward. Therefore, the proposed electrochemical immunosensor has wider application range than before. Under optimal conditions, the designed immunosensor exhibited a wide linear range from 1 pg mL−1 to 10 ng mL−1 with a low detection limit of 0.33 pg mL−1 (S/N = 3) for HIgG. The proposed immunosensor provides a promising application for the quantitative detection of biomolecules in serum samples.

An ultrasensitive sandwich-type electrochemical immunosensor based on the signal amplification system of double-deck gold film and thionine unite with platinum nanowire inlaid globular SBA-15 microsphere

A novel thionine unites with platinum nanowire inlaid globular SBA-15 (Pt NWs@g-SBA-15/Thi) not only utilizes as an efficient electrical signal probe but also constitutes an amplifying system with double-deck gold film (D-Au film) have been applied to the fabrication of sandwich-type immunosensor for detecting hepatitis B surface antigen (HBs Ag). The D-Au film can accelerate the electron transfer on the electrode interface due to the tunneling effect between the two Au films and can improve the load capacity of primary antibodies (Ab1) because of the good biocompatibility. The Pt NWs@g-SBA-15/Thi with uniform globular morphology not only can effectively reduce the spatial limitation for loading the secondary antibodies (Ab2) but also can provide outstanding pore accessibility of guest species from outside and offer catalytically active sites in a large scale. Besides, the presence of Thi can well enhance the electrical conductivity of Pt NWs@g-SBA-15/Thi. With the good cooperation between D-Au film and Pt NWs@g-SBA-15/Thi, a linear relationship between current signals and the concentrations of HBs Ag was obtained in the wide range from 10 fg/mL to 100ng/mL and the detection limit of HBs Ag was 3.3 fg/mL (signal-to-noise ratio of 3). Furthermore, the designed immunosensor with excellent selectivity, reproducibility and stability shows excellent performance in detection of human serum samples and provides a promising capacity for detecting a wide range of other tumor markers in clinical application.

Removal of Co(II) from aqueous solutions by sulfonated magnetic multi-walled carbon nanotubes

Sulfonated magnetic multi-walled carbon nanotubes (SMMWCNTs) were applied in the sorption of Co(II) from aqueous solutions. The SMMWCNTs were prepared and characterized by scanning electron microscope (SEM), Fourier transform infrared (FTIR), and X-ray diffractometer (XRD) test. A large number of influencing factors to the sorption process were investigated, such as pH, ionic strength, contact time, cations, anions, humic acid (HA), fulvic acid (FA) and temperature. The results indicated that the Co(II) sorption was strongly controlled by the pH and ionic strength. Moreover, foreign anions, such as F-, Cl- and Br-, had an obvious effect on the sorption process, which depended on the electronegativity of the anions. On the other hand, cations restrained sorption strongly, such as Mg2+ and Ca2+. The existence of HA/FA enhanced sorption process at pH<8 while weakened at pH>8. As revealed by the sorption results, the Langmuir adsorption model was more favorable than the Freundlich adsorption model, and the pseudo-second-order model could fit the data much better than the pseudo-first-order. The thermodynamic analysis suggested that sorption was spontaneous and endothermic. What’s more, the stability experiments of the SMMWCNTs showed that SMMWCNTs could maintain excellent magnetic stability and dispersion stability. Thus, this SMMWCNTs sorbent was believed to be a promising material for the selective removal of Co(II) from heavy metal-containing waste-water.