Jinhui Feng

Ultrasensitive amperometric immunosensor for PSA detection based on Cu2O@CeO2-Au nanocomposites as integrated triple signal amplification strategy.

In this work, a novel label-free electrochemical immunosensor was developed for the quantitative detection of prostate specific antigen (PSA). To this end, the amino functionalized cuprous oxide @ ceric dioxide (Cu2O@CeO2-NH2) core-shell nanocomposites were prepared to bond gold nanoparticles (Au NPs) by constructing stable Au-N bond between Au NPs and -NH2. Because the synergetic effect presents in Cu2O@CeO2 core-shell loaded with Au NPs (Cu2O@CeO2-Au), it shows better electrocatalytic activity towards the reduction of hydrogen peroxide (H2O2) than single Cu2O, Au NPs and Cu2O@CeO2. Featured by large specific surface area, good biocompatibility and good electrochemical properties which can greatly improve the electronic transmission rate, Cu2O@CeO2-Au was used as transducing materials to achieve efficiently capture antibodies and triple signal amplification of the proposed immunosensor. Under the optimal conditions, the proposed immunosensor exhibited a wide linear range from 0.1pg/mL to 100ng/mL with a low detection limit of 0.03pg/mL (S/N=3). Furthermore, the proposed label-free immunosensor has been used to determine PSA in human serum with satisfactory results. Meanwhile, it displayed good reproducibility, acceptable selectivity, and long-term stability, which had promising application in bioassay analysis.

Ultrasensitive electrochemical immunosensor for quantitative detection of SCCA using Co3O4@CeO2-Au@Pt nanocomposite as enzyme-mimetic labels

Recently early diagnosis of squamous cell carcinoma antigen (SCCA) as a tumor maker of various cancers has increasingly attracted a lot of attention with heightening of incidence rate of cancer. The SCCA with low concentration in human serum should be diluted before detecting. Thus, an immunoassay with high sensitivity is significant for early detecting SCCA. Therefore, a nonenzymatic sandwich-type electrochemical immunosensor herein was conducted to quantitative detection of squamous cell carcinoma antigen (SCCA). The amino functionalized cobaltosic oxide @ ceric dioxide nanocubes with core-shell morphology were prepared to combine sea-urchin like gold @ platinum nanoparticles (Co3O4@CeO2-Au@Pt), and used as labels to conjugate with secondary antibodies for signal amplification. Due to the synergetic effect, excellent electrochemical property and superior auxiliary catalytic activity of Co3O4@CeO2-Au@Pt, high electrocatalytic current responses toward the reduction of hydrogen peroxide (H2O2) were achieved. Besides, the electrodeposited gold nanoparticles (D-Au NPs) which were modified on glassy carbon electrodes (GCE) were used as antibodies carriers and sensing platforms. With the well cooperation of Co3O4@CeO2-Au@Pt and D-Au NPs, a broad linear range from 100fg/mL to 80ng/mL with a low detection limit of 33 fg/mL for detecting SCCA was achieved. In addition, the immunosensor displayed with good reproducibility, high selectivity and stability. The results are satisfactory when the proposed method has been applied to analyze human serum samples, indicating that the potential application is promising in clinical monitoring of tumor markers.

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.

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.

Sandwich-type electrochemical immunosensor based on Au@Ag supported on functionalized phenolic resin microporous carbon spheres for ultrasensitive analysis of α-fetoprotein

Signal amplification is crucial for obtaining low detection limits in electrochemical immunosensor. In this work, we developed a novel signal amplification strategy using Au@Ag nanoparticles loaded by polydopamine functionalized phenolic resin microporous carbon spheres (Au@Ag/PDA-PR-MCS). Phenolic resin microporous carbon spheres (PR-MCS) possesses uniform size and a large surface area (1656.8 m2 g-1). Polydopamine (PDA) functionalized phenolic resin microporous carbon spheres (PDA-PR-MCS) retains the advantages of PR-MCS and possesses strong adsorption ability. With the unique structure of PDA-PR-MCS, it not only improves the loading capacity and dispersity of Au@Ag nanoparticles (Au@Ag NPs), but also enhances the stability for the combination of the Au@Ag NPs by chemical absorption between Au@Ag NPs and -NH2 of PDA. The Au@Ag/PDA-PR-MCS exhibits extraordinary electrocatalytic activity towards reduction of hydrogen peroxide (H2O2) to make the electrochemical response more sensitive. Furthermore, Au NPs with good biocompatibility and excellent conductivity were electrodeposited on the surface of electrode, which was used as a sensing platform to immobilize primary antibody (Ab1) and accelerate the electron transfer on the electrode interface. Herein, the designed immunosensor provided a broad linear range from 20 fg/mL to 100 ng/mL for alpha fetoprotein (AFP) detection and a low detection limit of 6.7 fg/mL (signal-to-noise ratio of 3) under optimal experimental conditions. Moreover, the excellent performance in detection of human serum samples indicated that the proposed immunosensor will provide promising applications in clinical monitoring of AFP.

Facile synthesis of MoS2@Cu2O-Pt nanohybrid as enzyme-mimetic label for the detection of the Hepatitis B surface antigen

An ultrasensitive sandwich-type electrochemical immunosensor was proposed for quantitative detection of hepatitis B surface antigen, which is a representative biomarker of the Hepatitis B virus. First, the porous graphene oxide/Au composites with good conductive ability were employed to accelerate the electron transfer on the electrode interface. Furthermore, the amino functionalized molybdenum disulfide @ cuprous oxide hybrid with coral morphology was prepared to combine platinum nanoparticles for achieving signal amplification strategy. The resulting nanocomposites (molybdenum disulfide @ cuprous oxide - platinum) demonstrated uniform coral morphology, which effectively improved the specific surface area available for loading the secondary antibody and the number of catalytically active sites, even also increased the electrical conductivity. Based on these advantages, this composite system yielded a superior electrocatalytic current response toward the reduction of hydrogen peroxide. In addition, porous graphene oxide/Au composites were used to modify the glassy carbon electrode, thereby presenting a large surface area and becoming biocompatible, for improving the loading capacity of the primary antibody. Under optimal conditions, we obtained a linear relationship between current signal and hepatitis B surface antigen concentration in the broad range from 0.5pg/mL to 200ng/mL, with a detection limit of 0.15pg/mL (signal-to-noise ratio of 3). These values are promising towards clinical applications.

A sensitive non-enzymatic immunosensor composed of silver nanoflowers for squamous cell carcinoma antigen

In this work, a sensitive sandwich-type non-enzymatic electrochemical immunosensor for quantitative detection of squamous cell carcinoma antigen (SCCA) is designed and fabricated. Gold nanoparticles/graphene nanoribbons (Au NPs/NH2–GNRs) are used as the platform of electrochemical immunosensor to accelerate electron transfer and increase the specific surface area. The Au NPs with good biocompatibility can increase the probability of capturing primary antibodies (Ab1) to further improve the sensitivity. The silver nanoflower–molybdenum disulfide/multiwalled carbon nanotubes (SNFs–NH2–MoS2/MWCNTs) were used as labels of secondary antibodies (Ab2) and exhibit remarkable multiple-signal amplification effects. The silver nanoflowers with many branches can provide abundant active sites for the electrochemical reaction to further improve the sensitivity. Under the optimal conditions, the immunosensor shows a wide linear range between 0.1 pg mL−1 and 20 ng mL−1 with a limit of detection 0.03 pg mL−1. Furthermore, the novel immunosensor shows good performance for the detection of serum samples. The results indicate that the proposed immunosensor could be promising in the clinical application for quantitative detection of SCCA.

The label-free immunosensor based on rhodium@palladium nanodendrites/sulfo group functionalized multi-walled carbon nanotubes for the sensitive analysis of carcino embryonic antigen

In this work, bimetallic core-shell rhodium@palladium nanodendrites (Rh@Pd NDs) loaded on sulfo group functionalized multi-walled carbon nanotubes (MWCNTs-SO3H) were combined to form Rh@Pd NDs/MWCNTs-SO3H nanocomposites. And the composites were used to construct a simple and label-free electrochemical immunosensor for carcino embryonic antigen (CEA) detection using differential pulse voltammetry (DPV). Rh@Pd NDs with dendritic nanostructure not only provide abundant catalytically active sites, but also increase the loading of antibody, which could improve the analytical performance and result in high sensitivity. In addition, the MWCNTs-SO3H could further enhance electrochemical properties due to the excellent conductivity, good solubility and high surface area. Taking advantages of both Rh@Pd NDs and MWCNTs-SO3H, the proposed immunosensor showed a broad linear range from 25 fg mL-1 to 100 ng mL-1 for CEA detection and a low detection limit of 8.3 fg mL-1 (signal-to-noise ratio of 3) under optimal experimental conditions. Moreover, the expected immunosensor exhibited good reproducibility and high sensitivity, which could achieve excellent analysis of CEA in human serum with satisfactory results. Therefore, the Rh@Pd NDs/MWCNTs-SO3H nanocomposites may be considered as a sensing platform for fabrication of simple, ultrasensitive and label-free electrochemical immunosensor.

Ultrasensitive photoelectrochemical immunosensor of cardiac troponin I detection based on dual inhibition effect of Ag@Cu 2 O core-shell submicron-particles on CdS QDs sensitized TiO 2 nanosheets

Rapidity and high sensitivity are the critical factors for the diagnoses of heart attacks and cardiac troponin I (cTnI) is used as a gold standard marker for its diagnosis. To realize the accurate detection of cTnI, a novel ultrasensitive photoelectrochemical (PEC) immunosensor for cTnI determination was developed upon dual inhibition effect of Ag@Cu2O core-shell submicron-particles(SPs) toward CdS sensitized the (001) facets of anatase titanium dioxide nanosheets (TiO2/CdS). In this study, the TiO2/CdS composite not only indicated stable and excellent photoelectric signal but also provided abundant functional group to immobilized cTnI antibodies (Ab1). To obtain the high sensitivity, Ag@Cu2O core-shell SPs were used as labels of the secondary antibodies (Ab2), owning to competitive absorption of light and consumption of electron donor, less light energy and electron donors arrived at the TiO2/CdS sensitization structure. Besides, the remarkable steric hindrance effect of Ag@Cu2O core-shell SPs labeled secondary antibodies (Ab2) conjugates obstructed the transfer of electrons and diffusion of the electron donors to the photoelectrode surface, leading to further decrease of photocurrent. Therefore, the constructed immunosensor has an ultrasensitive response to cTnI in a liner range of 0.02 pg/mL to 50 ng/mL with a low detection limit of 6.7 fg/mL, and exhibits good sensitivity and admirable stability. Moreover, the strategy provided an efficient and novel approach for dual inhibition effect in PEC immunoassay development.