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1.
Graphene-CdS (G-CdS) nanocomposites were successfully prepared by CdS nanocrystals (CdS NCs) formed in situ on the surface of graphene sheets, using graphene oxide (GO) sheets with rich negatively charged carboxylic acid groups as starting materials. Compared with pure CdS NCs, the presence of the graphene doped in G-CdS nanocomposites could facilitate the electrochemical redox process of CdS NCs; further, the as-prepared G-CdS nanocomposite can react with H2O2 to generate strong and stable electrochemiluminescent (ECL) emission, which not only enhances its ECL intensity by about 4.3-fold but also decreases its onset potential for about 320 mV. The as-prepared solid-state ECL H2O2 sensor shows acceptable linear response from 5 μM up to 1 mM with a detection limit of 1.7 μM (S/N = 3). The ECL H2O2 sensor exhibits excellent reproducibility and long-term stability. Such a property would promote the potential application of the graphene as enhanced materials in fabricating sensors for chemical and biochemical analysis.  相似文献   

2.
Chen L  Lu L  Mo Y  Xu Z  Xie S  Yuan H  Xiao D  Choi MM 《Talanta》2011,85(1):56-62
Highly ordered titanium dioxide (TiO2) nanotubes film was successfully synthesized via anodic oxidation of a Ti foil in an ammonium fluoride-based ethylene glycol solution. The electrogenerated chemiluminescence (ECL) behavior of the resulting TiO2 nanotubes film was subsequently studied. Strong ECL emission was observed at −1.40 V (vs. Ag/AgCl) and the ECL spectrum displayed three emission peaks which were bathochromatically shifted by ca. 140 nm as compared to its corresponding photoluminescence (PL) emission peaks, indicating that the surface state plays an important role in the emission process. The ECL emission can also occur in a deareated solution attributing to the surface adsorbed O2 molecules. The ECL emission intensity was quenched by dopamine and greatly enhanced in the presence of dissolved O2 and H2O2, making it possible to detect these analytes. The TiO2 nanotubes film has been successfully applied to determine the dissolved O2 content in river and pond water samples, the H2O2 concentration in commercial disinfectant samples and the dopamine concentration in commercial dopamine injections with satisfactory results. The plausible ECL mechanisms of TiO2 nanotubes film in aqueous solution are discussed.  相似文献   

3.
Yongjin Zou  Lixian Sun  Fen Xu 《Talanta》2007,72(2):437-442
A Prussian Blue (PB)/polyaniline (PANI)/multi-walled carbon nanotubes (MWNTs) composite film was fabricated by step-by-step electrodeposition on glassy carbon electrode (GCE). The electrode prepared exhibits enhanced electrocatalytic behavior and good stability for detection of H2O2 at an applied potential of 0.0 V. The effects of MWNTs thickness, electrodeposition time of PANI and rotating rate on the current response of the composite modified electrode toward H2O2 were optimized to obtain the maximal sensitivity. A linear range from 8 × 10−9 to 5 × 10−6 M for H2O2 detection has been observed at the PB/PANI/MWNTs modified GCE with a correlation coefficient of 0.997. The detection limit is 5 × 10−9 M on signal-to-noise ratio of 3. To the best of our knowledge, this is the lowest detection limit for H2O2 detection. The electrode also shows high sensitivity (526.43 μA μM−1 cm−2) for H2O2 detection which is more than three orders of magnitude higher than the reported.  相似文献   

4.
A simple procedure has been used for preparation of modified glassy carbon electrode with carbon nanotubes and copper complex. Copper complex [Cu(bpy)2]Br2 was immobilized onto glassy carbon (GC) electrode modified with silicomolybdate, α-SiMo12O404− and single walled carbon nanotubes (SWCNTs). Copper complex and silicomolybdate irreversibly and strongly adsorbed onto GC electrode modified with CNTs. Electrostatic interactions between polyoxometalates (POMs) anions and Cu-complex, cations mentioned as an effective method for fabrication of three-dimensional structures. The modified electrode shows three reversible redox couples for polyoxometalate and one redox couple for Cu-complex at wide range of pH values. The electrochemical behavior, stability and electron transfer kinetics of the adsorbed redox couples were investigated using cyclic voltammetry. Due to electrostatic interaction, copper complex immobilized onto GC/CNTs/α-SiMo12O404− electrode shows more stable voltammetric response compared to GC/CNTs/Cu-complex modified electrode. In comparison to GC/CNTs/Cu-complex the GC/CNTs/α-SiMo12O404− modified electrodes shows excellent electrocatalytic activity toward reduction H2O2 and BrO3 at more reduced overpotential. The catalytic rate constants for catalytic reduction hydrogen peroxide and bromate were 4.5(±0.2) × 103 M−1 s−1 and 3.0(±0.10) × 103 M−1 s−1, respectively. The hydrodynamic amperommetry technique at 0.08 V was used for detection of nanomolar concentration of hydrogen peroxide and bromate. Detection limit, sensitivity and linear concentration range proposed sensor for bromate and hydrogen peroxide detection were 1.1 nM and 6.7 nA nM−1, 10 nM-20 μM, 1 nM, 5.5 nA nM−1 and 10 nM-18 μM, respectively.  相似文献   

5.
α-Fe2O3 nanoparticles prepared using a simple solution-combusting method have been dispersed in chitosan (CH) solution to fabricate nanocomposite film on glass carbon electrode (GCE). The as-prepared α-Fe2O3 nanoparticles were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM). The nanocomposite film exhibits high electrocatalytic oxidation for nitric oxide (NO) and reduction for hydrogen peroxide (H2O2). The electrocatalytic oxidation peak is observed at +0.82 V (vs. Ag/AgCl) and controlled by diffusion process. The electrocatalytic reduction peak is observed at −0.45 V (vs. Ag/AgCl) and controlled by diffusion process. This α-Fe2O3-CH/GCE nanocomposite bioelectrode has response time of 5 s, linearity as 5.0 × 10−7 to 15.0 × 10−6 M of NO with a detection limit of 8.0 × 10−8 M and a sensitivity of −283.6 μA/mM. This α-Fe2O3-CH/GCE nanocomposite bioelectrode was further utilized in detection of H2O2 with a detection limit of 4.0 × 10−7 M, linearity as 1.0 × 10−6 to 44.0 × 10−6 M and with a sensitivity of 21.62 μA/mM. The shelf life of this bioelectrode is about 6 weeks under room temperature conditions.  相似文献   

6.
Qian L  Yang X 《Talanta》2006,68(3):721-727
A new amperometric biosensor for hydrogen peroxide was developed based on cross-linking horseradish peroxidase (HRP) by glutaraldehyde with multiwall carbon nanotubes/chitosan (MWNTs/chitosan) composite film coated on a glassy carbon electrode. MWNTs were firstly dissolved in a chitosan solution. Then the morphology of MWNTs/chitosan composite film was characterized by field-emission scanning electron microscopy. The results showed that MWNTs were well soluble in chitosan and robust films could be formed on the surface. HRP was cross-linked by glutaraldehyde with MWNTs/chitosan film to prepare a hydrogen peroxide biosensor. The enzyme electrode exhibited excellent electrocatalytic activity and rapid response for H2O2 in the absence of a mediator. The linear range of detection towards H2O2 (applied potential: −0.2 V) was from 1.67 × 10−5 to 7.40 × 10−4 M with correction coefficient of 0.998. The biosensor had good repeatability and stability for the determination of H2O2. There were no interferences from ascorbic acid, glucose, citrate acid and lactic acid.  相似文献   

7.
Baiqing Yuan  Tianyan You 《Talanta》2009,79(3):730-1309
A novel tris(2,2′-bipyridine)ruthenium(II) (Ru(bpy)32+) cathodic electrochemiluminescence (ECL) was generated at −0.78 V at the Pt electrode in acetonitrile (ACN), which suggested that the cathodic ECL differed from conventional cathodic ECL. It was found that tripropylamine (TPrA) could enhance this cathodic ECL and the linear range (log-log plot) was 0.2 μM-0.2 mM. In addition, hydrogen peroxide (H2O2) could inhibit the cathodic ECL and was indirectly detected with the linear range of 27-540 μM. The RSD (n = 12) of the ECL intensity in the presence of 135 μM H2O2 was 0.87%. This method was also demonstrated for the fast determination of H2O2 in disinfectant sample and satisfactory results were obtained.  相似文献   

8.
In this paper, LaNi0.6Co0.4O3 (LNC) nanoparticles were synthesized by the sol–gel method, and the structure and morphology of LNC nanoparticles were characterized by X-ray diffraction spectrum, scanning electron microscopy and transmitting electron microscopy. And then, LNC was used to modify carbon paste electrode (CPE) without any adhesive to fabricate hydrogen peroxide and glucose sensor, and the results demonstrated that LNC exhibited strong electrocatalytical activity by cyclic voltammetry and amperometry. In H2O2 determination, linear response was obtained in the concentration range of 10 nM–100 μM with a detection limit of 1.0 nM. In glucose determination, there was the linear region of 0.05–200 μM with a detection limit of 8.0 nM. Compared with other reports, the proposed sensor also displayed high sensitivity toward H2O2 (1812.84 μA mM−1 cm−2) and glucose (643.0 μA mM−1 cm−2). Moreover, this prepared sensor was applied to detect glucose in blood serum and hydrogen peroxide in toothpaste samples with satisfied results, indicating its possibility in practical application.  相似文献   

9.
Qiu B  Xue L  Wu Y  Lin Z  Guo L  Chen G 《Talanta》2011,85(1):339-344
Inhibited Ru(bpy)32+ electrochemiluminescence by inorganic oxidants is investigated. Results showed that a number of inorganic oxidants can quench the ECL of Ru(bpy)32+/tri-n-propylamine (TPrA) system, and the logarithm of the decrease in ECL intensity (ΔI) was proportional to the logarithm of analyte concentrations. Based on which, a sensitive approach for detection of these inorganic oxidants was established, e.g. the log-log plots of ΔI versus the concentration of MnO4, Cr2O72− and Fe(CN)63− are linear in the range of 1 × 10−7 to 3 × 10−4 M for MnO4 and Cr2O72−, and 1 × 10−7 to 1 × 10−4 M for Fe(CN)63−, with the limit of detection (LOD) of 8.0 × 10−8 M, 2 × 10−8 M, and 1 × 10−8 M, respectively. A series of experiments such as a comparison of the inhibitory effect of different compounds on Ru(bpy)32+/TPrA ECL, ECL emission spectra, UV-Vis absorption spectra etc. were investigated in order to discover how these inorganic analytes quench the ECL of Ru(bpy)32+/TPrA system. A mechanism based on consumption of TPrA intermediate (TPrA·) by inorganic oxidants was proposed.  相似文献   

10.
A highly sensitive NOx sensor was designed and developed by electrochemical incorporation of copper nanoparticles (CuNP) on single-walled carbon nanotubes (SWCNT)-polypyrrole (PPy) nanocomposite modified Pt electrode. The modified electrodes were characterized by scanning electron microscopy and energy dispersive X-ray analysis. Further, the electrochemical behavior of the CuNP-SWCNT-PPy-Pt electrode was investigated by cyclic voltammetry. It exhibited the characteristic CuNP reversible redox peaks at −0.15 V and −0.3 V vs. Ag/AgCl respectively. The electrocatalytic activity of the CuNP-SWCNT-PPy-Pt electrode towards NOx is four-fold than the CuNP-PPy-Pt electrode. These results clearly revealed that the SWCNT-PPy nanocomposite facilitated the electron transfer from CuNP to Pt electrode and provided an electrochemical approach for the determination of NOx. A linear dependence (r2 = 0.9946) on the NOx concentrations ranging from 0.7 to 2000 μM, with a sensitivity of 0.22 ± 0.002 μA μM−1 cm−2 and detection limit of 0.7 μM was observed for the CuNP-SWCNT-PPy-Pt electrode. In addition, the sensor exhibited good reproducibility and retained stability over a period of one month.  相似文献   

11.
A series of spinel-type CoxNi1−xFe2O4 (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8, 1.0) magnetic nanomaterials were solvothermally synthesized as enzyme mimics for the eletroctrocatalytic oxidation of H2O2. X-ray diffraction and scanning electron microscope were employed to characterize the composition, structure and morphology of the material. The electrochemical properties of spinel-type CoxNi1−xFe2O4 with different (Co/Ni) molar ratio toward H2O2 oxidation were investigated, and the results demonstrated that Co0.5Ni0.5Fe2O4 modified carbon paste electrode (Co0.5Ni0.5Fe2O4/CPE) possessed the best electrocatalytic activity for H2O2 oxidation. Under optimum conditions, the calibration curve for H2O2 determination on Co0.5Ni0.5Fe2O4/CPE was linear in a wide range of 1.0 × 10−8–1.0 × 10−3 M with low detection limit of 3.0 × 10−9 M (S/N = 3). The proposed Co0.5Ni0.5Fe2O4/CPE was also applied to the determination of H2O2 in commercial toothpastes with satisfactory results, indicating that CoxNi1−xFe2O4 is a promising hydrogen peroxidase mimics for the detection of H2O2.  相似文献   

12.
In this paper, the electrogenerated chemiluminescence (ECL) from thiol-capped CdTe quantum dots (QDs) was reported. The ECL emission was occurred at −1.1 V and reached a maximum value at −2.4 V when the potential was cycled between 0.0 and −2.5 V. The reduced species of CdTe QDs could react with the coreactants to produce the ECL emission. The CdTe QD concentration (6.64 × 10−7 mol L−1) of ECL is lower than that (1.0 × 10−3 mol L−1) of chemiluminescence (CL). Based on the enhancement of light emission from thiol-capped CdTe QDs by H2O2 in the negative electrode potential, a novel method for the determination of H2O2 was developed. The light intensity was linearly proportional to the concentration of H2O2 between 2.0 × 10−7 and 1.0 × 10−5 mol L−1 with a detection limit of 6.0 × 10−8 mol L−1. Compared with most of previous reports, the proposed method has higher sensitivity for the determination of H2O2. In addition, the ECL spectrum of thiol-capped CdTe QDs exhibited a peak at around 620 nm, which was substantially red shifted from the photoluminescence (PL) spectrum, suggesting the surface states play an important role in this ECL process.  相似文献   

13.
In this paper, the highly intrinsic peroxidase-like catalytic activity of nitrogen-doped graphene quantum dots (N-GQDs) is revealed. This activity was greatly dependent on pH, temperature and H2O2 concentration. The experimental results showed that the stable N-GQDs could be used for the detection of H2O2 and glucose over a wide range of pH and temperature, offering a simple, highly selective and sensitive approach for their colorimetric sensing. The linearity between the analyte concentration and absorption ranged from 20 to 1170 μM for H2O2 and 25 to 375 μM for glucose with a detection limit of 5.3 μM for H2O2 and 16 μM for glucose. This assay was also successfully applied to the detection of glucose concentrations in diluted serum and fruit juice samples.  相似文献   

14.
A new electrochemiluminescent (ECL) detection system equipped with an electrically controlled heating cylindrical microelectrode (HME) was developed in this paper. The cylindrical microelectrode made of platinum wire (25 μm in diameter, 6 mm in long) was used as the working electrode of the ECL detection system, the temperature of the electrode could be controlled electrically. The Ru(bpy)32+-ECL and Ru(bpy)32+-C2O42−-ECL systems were used to evaluate this ECL detection system. The detection limit for oxalate was found to be 3.0 × 10−4 mol/L when Te (temperature of the HME) was 22 °C, and found to be 3.0 × 10−6 mol/L at 80 °C, which indicates that the detection limit can be improved greatly at higher Te, based on which, it is possible to establish a more sensitive method for measurement of ECL by using a heated microelectrode.  相似文献   

15.
A highly sensitive and stable tris(2,2′-bipyridyl)ruthenium(II) (Ru(bpy)32+) electrogenerated chemiluminescence (ECL) sensor was developed based on carbon nanotube (CNT) dispersed in mesoporous composite films of sol-gel titania and perfluorosulfonated ionomer (Nafion). Single-wall (SWCNT) and multi-wall carbon nanotubes (MWCNT) can be easily dispersed in the titania-Nafion composite solution. The hydrophobic CNT in the titania-Nafion composite films coated on a glassy carbon electrode certainly increased the amount of Ru(bpy)32+ immobilized in the ECL sensor by adsorption of Ru(bpy)32+ onto CNT surface, the electrocatalytic activity towards the oxidation of hydrophobic analytes, and the electronic conductivity of the composite films. Therefore, the present ECL sensor based on the CNT-titania-Nafion showed improved ECL sensitivity for tripropylamine (TPA) compared to the ECL sensors based on both titania-Nafion composite films without CNT and pure Nafion films. The present Ru(bpy)32+ ECL sensor based on the MWCNT-titania--Nafion composite gave a linear response (R2 = 0.999) for TPA concentration from 50 nM to 1.0 mM with a remarkable detection limit (S/N = 3) of 10 nM while the ECL sensors based on titania-Nafion composite without MWCNT, pure Nafion films, and MWCNT-Nafion composite gave a detection limit of 0.1 μM, 1 μM, and 50 nM, respectively. The present ECL sensor showed outstanding long-term stability (no signal loss for 4 months).  相似文献   

16.
Pentacyanoferrate-bound poly(1-vinylimidazole) (PVI[Fe(CN)5]) was selected as a mediator for amperometric creatinine determination based on the reductive H2O2 detection. Creatinine amidohydrolase (CNH), creatine amidohydrolase (CRH), sarcosine oxidase (SOD), peroxidase (POD), and PVI[Fe(CN)5] were crosslinked with poly(ethylene glycol) diglycidyl ether (PEGDGE) on a glassy carbon (GC) electrode for a creatinine biosensor fabrication. Reduction current was monitored at −0.1 V in the presence of creatinine and O2. It is revealed that PVI[Fe(CN)5] is suitable as a mediator for a bioelectrocatalytic reaction of POD, since PVI[Fe(CN)5] neither reacts with reactants nor works as an electron acceptor of SOD. The amounts of PVI[Fe(CN)5], PEGDGE, and enzymes were optimized toward creatinine detection. Nafion as a protecting film successfully prevented the enzyme layer from interferences. The detection limit and linear range in creatinine determination were 12 μM and 12–500 μM (R2 = 0.993), respectively, and the sensitivity was 11 mA cm−2 M−1, which is applicable for urine creatinine tests. The results of the creatinine determination for four urine samples measured with this proposed method were compared with Jaffe method, and a good correlation was obtained between the results.  相似文献   

17.
Hua MY  Chen HC  Tsai RY  Lai CS 《Talanta》2011,85(1):631-637
The imine of polybenzimidazole (PBI) is chemically oxidized by hydrogen peroxide (H2O2) in the presence of acetic acid (AcOH). Fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopies (XPS) showed that when the AcOH concentration remained constant, the degree of oxidation increased with increasing H2O2 levels. Moreover, the imine also exhibited electrochemical redox behavior. Based on these properties, a PBI-modified Au (PBI/Au) electrode was developed as an enzyme-free H2O2 sensor. At an applied potential of −0.5 V vs. Ag/AgCl, the current response of the PBI/Au electrode was linear with H2O2 concentration over a range from 0.075 to 1.5 mM, with a sensitivity of 55.0 μA mM−1 cm−2. The probe had excellent stability, with <5% variation from its initial response current after storage at 50 °C for 10 days. Potentially interfering species such as ascorbic or uric acid had no effect on sensitivity. Sensitivity improved dramatically when multiwalled carbon nanotubes (MWCNT) were incorporated in the probe. Under optimal conditions, the detection of H2O2 using a MWCNT-PBI/Au electrode was linear from 1.56 μM to 2.5 mM, with a sensitivity of 928.6 μA mM−1 cm−2. Analysis of H2O2 concentrations in urine samples using a MWCNT-PBI/Au electrode produced accurate real-time results comparable to those of traditional HPLC methods.  相似文献   

18.
In this paper, a novel sandwich electrochemiluminescence (ECL) immunosensor was constructed by ferrocene for quenching Ag nanoparticles functionalized g-C3N4 (Ag@g-C3N4) emission. The prepared Ag@g-C3N4 had strong and stable ECL signals compared to pure g-C3N4 and primary antibody (Ab1) can be immobilized on Ag@g-C3N4 by adsorption of Ag nanoparticles. Ferrocene carboxylic acid (Fc-COOH) labeled secondary antibody was immobilized on Au doped mesoporous Al2O3 nanorods (Au@Al2O3–Fc-COOH@Ab2) as labels through adsorption ability of Au toward proteins. After a sandwich-type immunoreaction, a remarkable decrease of ECL signal was observed due to the ECL quenching of Ag@g-C3N4 by Au@Al2O3–Fc-COOH@Ab2. As a result, the change of ECL intensity has a direct relationship with the logarithm of CEA concentrations in the range of 1 pg mL−1–100 ng mL−1 with a detection limit of 0.35 pg mL−1 (S/N = 3). Additionally, the proposed immunosensor shows high specificity, good reproducibility, and long-term stability.  相似文献   

19.
Iron oxide modified with single- or double-metal additives (Cr, Ni, Zr, Ag, Mo, Mo-Cr, Mo-Ni, Mo-Zr and Mo-Ag), which can store and supply pure hydrogen by reduction of iron oxide with hydrogen and subsequent oxidation of reduced iron oxide with steam (Fe3O4 (initial Fe2O3)+4H2↔3Fe+4H2O), were prepared by impregnation. Effects of various metal additives in the samples on hydrogen production were investigated by the above-repeated redox. All the samples with Mo additive exhibited a better redox performance than those without Mo, and the Mo-Zr additive in iron oxide was the best effective one enhancing hydrogen production from water decomposition. For Fe2O3-Mo-Zr, the average H2 production temperature could be significantly decreased to 276 °C, the average H2 formation rate could be increased to 360.9-461.1 μmol min−1 Fe-g−1 at operating temperature of 300 °C and the average storage capacity was up to 4.73 wt% in four cycles, an amount close to the IEA target.  相似文献   

20.
A new method for uric acid (UA) determination based on the quenching of the cathodic ECL of the tris(2,2-bipyridine)ruthenium(II)–uricase system is described. The biosensor is based on a double-layer design containing first tris(2,2-bipyridine)ruthenium(II) (Ru(bpy)32+) electrochemically immobilized on graphite screen-printed cells and uricase in chitosan as a second layer. The uric acid biosensing is based on the ECL quenching produced by uric acid over the cathodic ECL caused by immobilized Ru(bpy)32+ in the presence of uricase. The use of a −1.1 V pulse for 1 s with a dwelling time of 10 s makes it possible to estimate the initial enzymatic rate, which is used as the analytical signal. The Stern–Volmer type calibration function shows a dynamic range from 1.0 × 10−5 to 1.0 × 10−3 M with a limit of detection of 3.1 × 10−6 M and an accuracy of 13.6% (1.0 × 10−4 M, n = 5) as relative standard deviation. Satisfactory results were obtained for urine samples, creating an affordable alternative for uric acid determination.  相似文献   

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