Malik Saddam Khan

Label-free photoelectrochemical immunoassay for CEA detection based on CdS sensitized WO3@BiOI heterostructure nanocomposite

In this work, a label-free photoelectrochemical (PEC) immunosensor for the detection of carcino embryonic antigen (CEA) was developed based on CdS nanowires (NWs) sensitized WO3@BiOI heterostructure. The construction procedure of ITO/WO3@BiOI@CdS electrode was done by dipping the WO3@BiOI modified indium-tin oxide (ITO) electrode interchangeably into [Cd(NH3)4]2+ and S2- solution for several times. Then the ITO/WO3@BiOI@CdS electrode was used as a matrix for the subsequent immobilization of CEA antibody (Ab). The obtained label-free PEC immunosensor showed an excellent PEC performance toward CEA detection. Under optimal conditions, the PEC immunosensor have a sensitive response to CEA in a liner range of 0.01ng/mL to 50ng/mL with a detection limit of 3.2pg/mL. The proposed PEC immunosensor exhibited good stability, high sensitivity as well as reproducibility and storage stability. Moreover, the obtained PEC immunosensor also showed a satisfied result in human serum sample analysis.

Macroporous graphene capped Fe3O4 for amplified electrochemiluminescence immunosensing of carcinoembryonic antigen detection based on CeO2@TiO2

A novel electrochemiluminescence (ECL) signal-amplified immunosensing strategy was proposed by using gold nanoparticles (Au NPs) functionalized reduced graphene oxide (rGO) capped Fe3O4 (Au-FrGO). In this work, CeO2@TiO2 was prepared by a sol-gel method to wrap CeO2 with TiO2. In the presence of CeO2, CeO2@TiO2 exhibited better ECL activity than TiO2 with peroxydisulfate as coreactant. In addition, FrGO with macroporous structure was synthesized by self-assembly of rGO sheets capped cationic Fe3O4 nanoparticles, exhibiting larger specific surface area than rGO. Due to the low toxicity and magnetism of Fe3O4, FrGO owned more favorable biocompatibility and the application of magnetic-separation simplified the preparation procedure. After hybridizing with Au NPs, FrGO exhibited more excellent electrical conductivity and could immobilize more CeO2@TiO2 and antibodies. Therefore, a novel label-free ECL immunosensor based on Au-FrGO-CeO2@TiO2 was constructed which generated higher ECL response. To investigate the performance of the immunosensor, carcinoembryonic antigen (CEA) was chosen as a model target analyte. Under optimal conditions, the immunosensor had sensitive response to CEA in a wide linear range of 0.01pgmL-1 to 10ngmL-1 with a detection limit of 3.28 fg mL-1. The proposed ECL immunosensor exhibited excellent stability, repeatability and selectivity, which opened another promising avenue for CEA determination in real serum samples.

An ultrasensitive photoelectrochemical immunosensor for insulin detection based on BiOBr/Ag2S composite by in-situ growth method with high visible-light activity

A novel ultrasensitive label-free immunosensor based on BiOBr/Ag2S composite with high visible-light photoelectrochemical activity was prepared for the detection of insulin. After BiOBr was modified by thioglycolic acid, Ag2S nanoparticles were grown in-situ on the surface of BiOBr hierarchical microspheres to first form novel BiOBr/Ag2S composite. When ascorbic acid (AA) was used as an efficient electron donor for scavenging photo-generated holes, BiOBr/Ag2S composite material showed excellent photoelectrochemical activity. In order to immobilize insulin antibody, adhesive polydopamine (PDA) film formed by self-polymerization of dopamine was fabricated onto BiOBr/Ag2S modified electrode. Moreover, PDA film could further enhance the visible light absorption of BiOBr/Ag2S. When the solutions of 0.08molL-1AgNO3 and 0.1molL-1 AA were selected respectively during fabrication and detection process of this sensor, the best photocurrent singles were obtained. Under the optimum experimental condition, the specific binding between insulin and antibody resulted in a decrease in photocurrent intensity and the intensity decreased linearly with the logarithm of insulin concentration in the range of 0.001-20ngmL-1 with a detection limit of 0.2pgmL-1. The photoelectrochemical sensor ITO/BiOBr/Ag2S/PDA/anti-Insulin/BSA/Insulin revealed facile preparation, high sensitivity, and acceptable reproducibility, which may have practical applications in the biosensor, clinical diagnosis of cancers, photocatalysis, and other related fields.

Zinc-doping enhanced cadmium sulfide electrochemiluminescence behavior based on Au-Cu alloy nanocrystals quenching for insulin detection

Novel and sensitive sandwich-type electrochemiluminescence (ECL) immunosensor was fabricated for insulin detection. Au-ZnCd14S combined nitrogen doping mesoporous carbons (Au-ZnCd14S/NH2-NMCs) acted as sensing platform and Au-Cu alloy nanocrystals were employed as labels to quench the ECL of Au-ZnCd14S/NH2-NMCs. Zinc-doping promoted the ECL behavior of CdS nanocrystals, with the best ECL emission obtained when the molar ratio of Zn/Cd was 1:14. Simultaneously, the modification of gold nanoparticles (Au NPs) and combination with NH2-NMC further enhanced the ECL emission of ZnCd14S due to its excellent conductivity and large specific surface area, which is desirable for the immunosensor construction. Au-Cu alloy nanocrystals were employed in the ECL system of ZnCd14S/K2S2O8 triggering ECL quenching effects. The ECL spectra of ZnCd14S, acting as the energy donor, exhibited well overlaps with the absorption band of Au-Cu alloy nanocrystals which acted as the energy acceptor, leading to an effective ECL resonance energy transfer (ECL-RET). On the basis of the ECL quenching effects, a sensitive ECL immunosensor for insulin detection was successfully constructed with a linear response range of insulin concentration from 0.1pg/mL to 30ng/mL and the limit of detection was calculated to be 0.03pg/mL (S/N = 3).

A bio-chemical application of N-GQDs and g-C3N4 QDs sensitized TiO2 nanopillars for the quantitative detection of pcDNA3-HBV

Herein, TiO2 nanopillars (NPs)/N-doped graphene quantum dots (N-GQDs)/g-C3N4 QDs heterojunction efficiently suppressed the photogenerated charges recombination and improved photo-to-current conversion efficiency. The introduced N-GQDs and g-C3N4 QDs could result in more effective separation of the photogenerated charges, and thus produce a further increase of the photocurrent. TiO2 NPs/N-GQDs/g-C3N4 QDs were firstly applied as the photoactive materials for the fabrication of the biosensors, and the primers of pcDNA3-HBV were then adsorbed on the TiO2 NPs/N-GQDs/g-C3N4 QDs modified electrode under the activation of EDC/NHS. With increase of the pcDNA3-HBV concentration, the photocurrent reduced once the double helix between the primers and pcDNA3-HBV formed. The developed photoelectrochemical (PEC) biosensor showed a sensitive response to pcDNA3-HBV in a linear range of 0.01 fmol/L to 20nmol/L with a detection limit of 0.005 fmol/L under the optimal conditions. The biosensor exhibited high sensitivity, good selectivity, good stability and reproducibility.

Visible-light driven Photoelectrochemical Immunosensor Based on SnS 2 @mpg-C 3 N 4 for Detection of Prostate Specific Antigen

Herein, a novel label-free photoelectrochemical (PEC) immunosensor based on SnS2@mpg-C3N4 nanocomposite is fabricated for the detection of prostate specific antigen (PSA) in human serum. Firstly, mesoporous graphite-like carbon nitride (mpg-C3N4) with carboxyl groups is synthesized successfully which possesses high specific surface area and large pore volume. Then, SnS2 as a typical n-type semiconductor with weak photoelectric conversion capability is successfully loaded on carboxylated mpg-C3N4 to form a well-matched overlapping band-structure. The as-synthesized SnS2@mpg-C3N4 nanocomposite performs outstanding photocurrent response under visible-light irradiation due to low recombination rate of photoexcited electron-hole pairs, which is transcend than pure SnS2 or pure mpg-C3N4. It is worth noting that SnS2@mpg-C3N4 nanocomposite is firstly employed as the photoactive material in PEC immunosensor area. The concentration of PSA can be analyzed by the decrease in photocurrent resulted from increased steric hindrance of the immunocomplex. Under the optimal conditions, the developed PEC immunosensor displays a liner photocurrent response in the range of 50 fg·mL−1 ~ 10 ng·mL−1 with a low detection limit of 21 fg·mL−1. Furthermore, the fabricated immunosensor with satisfactory stability, reproducibility and selectivity provides a novel method for PSA determination in real sample analysis.

Ni(OH)2/NGQDs-based electrochemiluminescence immunosensor for prostate specific antigen detection by coupling resonance energy transfer with Fe3O4@MnO2 composites

An efficient quenching electrochemiluminescence (ECL) immunosensor based on ECL resonance energy transfer (ECL-RET) was studied for sensitive analysis of prostate specific antigen (PSA). In this protocol, nitrogen-doped graphene quantum dots (NGQDs) which could produce excellent ECL emission, were loaded onto Ni(OH)2 with the three-dimensional (3D) hierarchical and stacked lamellar structure. Taking advantages of high conductivity and large specific surface area of Ni(OH)2, the better electrochemical and ECL behavior of Ni(OH)2/NGQDs were presented. As another part of immunosensor, the Fe3O4@MnO2 composites with wider ultraviolet absorption range were successfully assembled. The absorption spectra of Fe3O4@MnO2 precisely overlapped with the ECL spectra of NGQDs, leading to the significant decrement of ECL signal. Herein, the sandwich-type immunosensor was developed based on the quenching mechanism between NGQDs (ECL donor) and Fe3O4@MnO2 (ECL acceptor). The system was optimized to realize reliable determination of PSA concentration within the linear range of 10-5-10ng/mL and a detection limit of 5 fg/mL (S/N = 3). Eminently, the developed method was successfully applied in real serum samples with good recoveries in a range from 94.0% to 102%, indicating the good accuracy of the proposed method for PSA detection.

A novel label-free photoelectrochemical sensor based on N,S-GQDs and CdS co-sensitized hierarchical Zn 2 SnO 4 cube for detection of cardiac troponin I

A novel label-free photoelectrochemical (PEC) sensor based on graphene quantum dots doped with nitrogen and sulfur (N,S-GQDs) and CdS co-sensitized hierarchical Zn2SnO4 cube was fabricated to detect cardiac troponin I (cTnI). The unique hierarchical Zn2SnO4 cube was synthesized successfully by the solvothermal method, which has a large specific surface to load functional materials. N,S-GQDs nanoparticles were assembled to the surface of cubic Zn2SnO4 coated ITO electrode, which efficiently accelerated the electronic transition and improved photo-to-current conversion efficiency. Then, CdS nanoparticles further were modified by in-situ growth method to form Zn2SnO4/N,S-GQDs/CdS composite with prominent photocurrent, which was 30 times that of the Zn2SnO4 cube alone. In this work, the specific immune recognition between cTnI antigens and cTnI antibodies (anti-cTnI) reduced the intensity of the photoelectric signal. And the intensity decreased linearly with the logarithm of cTnI concentration range from 0.001 ng/mL to 50 ng/mL with a detection limit of 0.3 pg/mL. With high sensitivity, excellent selectivity, good stability and reproducibility, the fabricated PEC sensor showed promising applications in the sensor, clinical diagnosis of myocardial infarction and PEC analysis.

Biosorption performance evaluation of heavy metal onto aerobic granular sludge-derived biochar in the presence of effluent organic matter via batch and fluorescence approaches

In present study, the biosorption process of Cu(II) onto aerobic granular sludge-derived biochar was evaluated in the absence and presence of effluent organic matter (EfOM) by using batch and fluorescence approaches. It was found that EfOM gave rise to enhancement of Cu(II) removal efficiency onto biochar, and the sorption data were better fitted with pseudo-second order model and Freundlich equation, in despite of the absence and presence of EfOM. According to excitation-emission matrix (EEM), EfOM was mainly comprised by humic-like substances and fulvic-like substances and their intensities were reduced in the addition of biochar and Cu(II) from batch biosorption process. Synchronous fluorescence spectra coupled to two-dimensional correlation spectroscopy (2D-COS) further implied that a successive fluorescence quenching was observed in various EfOM fractions with the increasing Cu(II) concentration. Moreover, fulvic-like fraction was more susceptibility than other fractions for fluorescence quenching of EfOM.

Dual-responsive electrochemical immunosensor for detection of insulin based on dual-functional zinc silicate spheres-palladium nanoparticles

In this study, described an electrochemical immunoassay for insulin that is based on the use of zinc silicate spheres loaded with palladium nanoparticles (Zn2SiO4-PdNPs) that act as dual-function labels. The Zn2SiO4-PdNPs display high electrocatalytic activity towards the reduction of H2O2 and high sensitivity in chronoamperometry. The Zn2SiO4-PdNPs decrease the electron transfer rate between the electrolyte and the surface of the electrode, which can increase the changed current and enhance the sensitivity of the immunosensor as detected by square wave voltammetry (SWV). Electrodeposited gold is used as the matrix material. The icosahedral gold nanocrystals are coated with the primary antibodies formed a 3D mode to against abundant of insulin. Under optimal conditions, the assay has a linear response in the 0.1pgmL-1 to 50ngmL-1 insulin concentration range, and the limit of detection of the SWV and CA methods are 0.25 fg mL-1 and 80 fg mL-1, respectively. Moreover, the immunosensor holds an outstanding analytical performance for the insulin detection and has promising potential in clinical diagnosis.