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1.
Because of its high activity and selectivity toward the reduction of hydrogen peroxide and oxygen, Prussian blue (PB) is usually considered as an “artificial enzyme peroxidase” and has been extensively used in the construction of electrochemical biosensors. In this study, we report on the construction of amperometric biosensors via grafting PB nanoparticles on the polymeric matrix of multiwalled carbon nanotubes (MWCNTs) and poly(4‐vinylpyridine) (PVP). The MWCNT/PVP/PB composite films were synthesized by casting films of MWCNTs wrapped with PVP on gold electrodes followed by electrochemical deposition of PB on the MWCNT/PVP matrix. The electrode modified with the MWCNT/PVP/PB composite film shows prominent electrocatalytic activity toward the reduction of hydrogen peroxide, which can be explained by the remarkable synergistic effect of the MWCNTs and PB. Therefore, fast amperometric response of this sensor to hydrogen peroxide was observed with a detection sensitivity of 1.3 μA μM –1 of H2O2 per square centimeter area and a detection limit of 25 nM . These results are much better than those reported for PB‐based amperometric sensors. In addition, a glucose biosensor fabricated by casting an additional glucose oxidase (GOD) containing Nafion film above the MWCNT/PVP/PB composite film shows promise for the sensitive and fast detection of glucose. The observed high stability, high sensitivity, and high reproducibility of the MWCNT/PVP/PB composite films make them promising for the reliable and durable detection of hydrogen peroxide and glucose.  相似文献   

2.
A novel nonenzymatic immunosensor for sensitive detection of Microcystin‐LR (MC‐LR) is constructed using a graphene platform combined with mesoporous PtRu alloy as a label for signal amplification. Primary antibody‐Microcystin‐LR (Ab1) is immobilized onto the surface of a graphene sheet (GS) through an amidation reaction between the carboxylic acid groups attached to the GS and the available amine groups of Ab1. Mesoporous PtRu alloy, prepared by corrosion PtRuAl alloys, is employed as a label to immobilize secondary antibody (Ab2). The resulting nanoparticles, PtRu‐Ab2, are used as labels for the immunosensor to detect MC‐LR. Under optimal conditions, the immunosensor exhibits a wide linear response to MC‐LR that ranges from 0.01 to 28 ng·mL?1, with a low detection limit of 9.63 pg·mL?1 MC‐LR. The proposed immunsensor shows good reproducibility, selectivity, and stability. The assayed results of polluted water with the sandwich‐type sensor are acceptable. Importantly, this methodology may provide a promising ultrasensitive assay strategy for other environmental pollutants.  相似文献   

3.
Direct glucose sensing on highly ordered platinum‐nanotubule array electrodes (NTAEs) is systematically investigated. The NTAEs are fabricated by electrochemical deposition of platinum in a 3‐aminopropyltrimethoxysilane‐modified anodic alumina membrane. Their structures and morphologies are then characterized using X‐ray diffraction and scanning electron microscopy, respectively. Electrochemical results show that NTAEs with different real surface areas could be achieved by controlling the deposition time or by using anodic alumina membranes with different pore size. Electrochemical responses of the as‐synthesized NTAEs to glucose in a solutions of either 0.5 M H2SO4, or phosphate‐buffered saline (PBS, pH 7.4) containing 0.1 M KCl are discussed. Based on the different electrochemical reaction mechanisms of glucose and interferents such as p‐acetamedophenol and ascorbic acid, their high roughness factor makes NTAEs sensitive, selective, and stable enough to be a kind of biosensor for the non‐enzymatic detection of glucose. Such a glucose sensor allows the determination of glucose in the linear range 2–14 mM, with a sensitivity of 0.1 μA cm–2 mM–1 (correlation coefficient 0.999), and a detection limit of 1.0 μM glucose, with neglectable interference from physiological levels of 0.1 mM p‐acetamedophenol, 0.1 mM ascorbic acid, and 0.02 mM uric acid.  相似文献   

4.
A facile one‐step printing process by 3D micro‐extrusion affording binder‐free thermally reduced graphene oxide (TRGO) based electrochemical capacitors (ECs) that display high‐rate performance is presented. Key intermediates are binder‐free TRGO dispersion printing inks with concentrations up to 15 g L?1. This versatile printing technique enables easy fabrication of EC electrodes, useful in both aqueous and non‐aqueous electrolyte systems. The as‐prepared TRGO material with high specific surface area (SSA) of 593 m2 g?1 and good electrical conductivity of ≈16 S cm?1 exhibits impressive charge storage performances. At 100 and 120 Hz, ECs fabricated with TRGO show time constants of 2.5 ms and 2.3 ms respectively. Very high capacitance values are derived at both frequencies ranging from 3.55 mF cm?2 to 1.76 mF cm?2. Additionally, these TRGO electrodes can be charged and discharged at very high voltage scan rates up to 15 V s?1 yielding 4 F cm?3 with 50% capacitance retention. Electrochemical performance of TRGO electrodes in electrolyte containing tetraethyl ammonium tetrafluoroborate and acetonitrile (TEABF4‐ACN) yields high energy density of 4.43 mWh cm?3 and power density up to 42.74 kW cm?3, which is very promising for AC line filtering application and could potentially substitute state of the art electrolytic capacitor technology.  相似文献   

5.
Chemical modification with foreign atoms is a leading strategy to intrinsically modify the properties of host materials. Among them, potassium (K) modification plays a critical role in adjusting the electronic properties of carbon materials. Graphene, a true 2D carbon material, has shown fascinating applications in electrochemical sensing and biosensing. In this work, a facile and mild strategy to K‐modifying in graphene at room‐temperature is reported for the first time. X‐ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), transmission electron microscopy (TEM), Raman spectra, and cyclic voltammetry are used to characterize this K‐modified graphene. The K‐modified graphene is capable of acting as an electron transfer medium and more efficiently promotes charge transfer than unmodified graphene. A highly sensitive and stable amperometric sensor based on its excellent electrocatalytic activity toward the oxidation of NO2? is proposed. The sensor shows a linear range from 0.5 μM to 7.8 mM with a detection limit of 0.2 μM at a signal‐to‐noise ratio of 3. The modified electrode has excellent analytical performance and can be successfully applied in the determination of NO2? released from liver cancer and leukemia cells and shows good application potential in biological systems.  相似文献   

6.
Graphdiyne (GDY), an emerging type of carbon allotropes, possesses fascinating electrical, chemical, and mechanical properties to readily spark energy applications in the realm of Li‐ion and Na‐ion batteries. Nevertheless, rational design of GDY architectures targeting advanced K‐ion storage has rarely been reported to date. Herein, the first example of synthesizing GDY frameworks in a scalable fashion to realize superb potassium storage for high‐performance K‐ion battery (KIB) anodes is showcased. To begin with, first principles calculations provide theoretical guidances for analyzing the intrinsic potassium storage capability of GDY. Meanwhile, the specific capacity is predicted to be as high as 620 mAh g?1, which is considerably augmented as compared with graphite (278 mAh g?1). Experimental tests then reveal that prepared GDY framework indeed harvests excellent electrochemical performance as a KIB anode, achieving high specific capacity (≈505 mAh g?1 at 50 mA g?1), outstanding rate performance (150 mAh g?1 at 5000 mA g?1) and favorable cycling stability (a high capacity retention of over 90% after 2000 cycles at 1000 mA g?1). Furthermore, kinetic analysis reveals that capacitive effect mainly accounts for the K‐ion storage, with operando Raman spectroscopy/ex situ X‐ray photoelectron spectroscopy identifying good electrochemical reversibility of GDY.  相似文献   

7.
The utilization of iron‐based species (mainly metallic iron, hematite and magnetite) encapsulated into multi‐walled carbon nanotubes (CNTs) as reactants in an electrochemical synthesis is reported for the first time in this work. Prussian blue (PB) is electrosynthesized in a heterogeneous reaction between ferricyanide ions in aqueous solution and the iron‐species encapsulated into CNTs, resulting in novel CNT/PB paste electrodes. This innovative preparation route produces an intimate contact between the PB and the CNTs, which improves the stability and redox properties of PB. The PB formation and the chemical interaction between the PB and the CNTs are confirmed by Raman spectroscopy. The electrode is employed as a hydrogen peroxide amperometric sensor, resulting in a very low limit of detection (1.94 × 10?8 mol L?1) and very high sensitivity (15.3 A cm?2 M ?1).  相似文献   

8.
A novel nanoparticle label capable of amplifying the electrochemical signal of DNA hybridization is fabricated by functionalizing poly(styrene‐co‐acrylic acid) microbeads with CdTe quantum dots. CdTe‐tagged polybeads are prepared by a layer‐by‐layer self‐assembly of the CdTe quantum dots (diameter = 3.07 nm) and polyelectrolyte on the polybeads (diameter = 323 nm). The self‐assembly procedure is characterized using scanning and transmission electron microscopy, and X‐ray photoelectron, infrared and photoluminescence spectroscopy. The mean quantum‐dot coverage is (9.54 ± 1.2) × 103 per polybead. The enormous coverage and the unique properties of the quantum dots make the polybeads an effective candidate as a functionalized amplification platform for labelling of DNA or protein. Herein, as an example, the CdTe‐tagged polybeads are attached to DNA probes specific to breast cancer by streptavidin–biotin binding to construct a DNA biosensor. The detection of the DNA hybridization process is achieved by the square‐wave voltammetry of Cd2+ after the dissolution of the CdTe tags with HNO3. The efficient carrier‐bead amplification platform, coupled with the highly sensitive stripping voltammetric measurement, gives rise to a detection limit of 0.52 fmol L?1 and a dynamic range spanning 5 orders of magnitude. This proposed nanoparticle label is promising, exhibits an efficient amplification performance, and opens new opportunities for ultrasensitive detection of other biorecognition events.  相似文献   

9.
A streptavidin‐functionalized silver‐nanoparticle‐enriched carbon nanotube (CNT/Ag NP) is designed as trace tag for ultrasensitive multiplexed measurements of tumor markers using a disposable immunosensor array. The CNT/Ag NP nanohybrid is prepared by one‐pot in situ deposition of Ag NPs on carboxylated CNTs. The nanohybrid is functionalized with streptavidin via the inherent interaction between the protein and Ag NPs for further linkage of biotinylated signal antibodies to obtain tagged antibodies. The functionalization process greatly improves the dispersibility of the nanohybrid in water. The immunosensor array is prepared by covalently immobilizing capture antibodies on chitosan‐modified screen‐printed carbon electrodes. Through a sandwich‐type immunoreaction on the immunosensor array, numerous Ag NPs are captured onto every single immunocomplex and are further amplified by a subsequent Ag NP‐promoted deposition of silver from a silver enhancer solution to obtain the sensitive electrochemical‐stripping signal of the Ag NPs. Using carcinoembryonic antigen and α‐fetoprotein as model analytes, this proposed multiplexed immunoassay method shows acceptable precision and wide linear ranges over four orders of magnitude with detection limits down to 0.093 and 0.061 pg mL?1, respectively. The assay results of serum samples with the proposed method are in acceptable agreement with the reference values. The newly designed strategy and the functionalized tag avoid cross‐talk and the requirement of deoxygenation for electrochemical immunoassay, and thus provide a promising potential in clinical application.  相似文献   

10.
Development of low cost electrocatalysts with outstanding catalytic activity and stability for oxygen evolution reaction (OER) in acid is a major challenge to produce hydrogen energy from water splitting. Herein, a novel metal‐free electrocatalyst consisting of a oxygen‐functionalized electrochemically exfoliated graphene (OEEG) nanosheets array is reported. Benefitting from a vertically aligned arrays structure and introducing oxygen functional groups, the metal‐free OEEG nanosheets array exhibits superior electrocatalytic activity and stability toward OER with a low overpotential of 334 mV at 10 mA cm?2 in acidic electrolyte. Such a high OER performance is thus far the best among all previously reported metal‐free carbon‐based materials, and even superior to commercial Ir/C catalysts (420 mV at 10 mA cm?2) in acid. Characterization results and electrochemical measurements identify the COOH species in the OEEG acting as active sites for acidic OER, which is further supported by atomic‐scale scanning transmission electron microscopy imaging and electron energy‐loss spectroscopy. Density functional theory calculations reveal that the reaction pathway of dual sites that is mixed by zigzag and armchair edges (COOH‐zig‐corner) is better than the pathway of single site.  相似文献   

11.
Morphology reshaping or reconfiguration, a concept widely used in plastic surgery, energy harvesting, and reconfigurable robots, is introduced for the first time to construct densified electrodes and realize compact Li‐ion storage desirable for high specific energy storage field. Hausmannite‐based hybrid materials, as a proof‐of‐concept prototype, engineered by 1‐methyl‐2‐pyrrolidinone‐soluble surface/interface organic encapsulation, which is crucial in reshaping, exhibit a remarkable increase in the volumetric capacity of more than five times after this process (≈1889 Ah L?1 vs ≈322 Ah L?1). With the simultaneous maintenance of the intrinsic nature, good contact, and no collapsed/agglomerated unit structures of the materials in electrodes, the design affords a maximal increase in the packing compactness and manifests no sacrifice of the reversible ion storage capability (1150 mAh g?1 at 40 mA g?1), stable cycling (≈100% capacity retention), high rate performance (185 mAh g?1 at 10 A g?1), and long lifespan (1000 cycles with 108% capacity retention, ≈455 mAh g?1 at 3 A g?1) for relatively highly loaded electrodes (active materials: 1.20–5.34 mg cm?2). The concept may not only shed new light on fabricating advanced Si‐based and other high capacity–related densified Li storage electrodes but also inject fresh vitality into the field of high‐density power sources.  相似文献   

12.
Microsupercapacitors (MSCs) with neutral multivalent electrolytes are safer, cheaper, and exhibit higher theoretical energy densities compared with the MSCs with acidic and alkaline electrolytes. Multivalent charge carriers (e.g., Mg2+, Zn2+) in the MSCs with Ti3C2Tx MXene electrodes have not been demonstrated, which could theoretically achieve higher specific capacitances and energy densities. However, because of the larger size of multivalent charge carriers, the MXene electrodes require further modifications to facilitate reversible electrochemical reactions. Herein, through spontaneous intercalation of various metal ions into MXene multilayers, twelve metal ion intercalated MXene electrodes (Mn+‐MXene) are fabricated and demonstrate improved electrochemical performance. Different nanopillar effects are observed between divalent Be2+ and trivalent Al3+ intercalants, which are systematically investigated by electrochemical impedance spectroscopy and molecular dynamics simulation. Among all Mn+‐MXene electrodes, the Be2+‐MXene electrode largely facilitates the charge‐transfer process with minimal disturbance of electrolyte diffusion rates, showing improved specific capacitances and high rate performance in univalent (Li2SO4, Na2SO4, K2SO4) and multivalent electrolytes (BeSO4, MgSO4, ZnSO4). Finally, flexible Be2+‐MXene MSCs with neural ZnSO4 gel electrolytes are fabricated, demonstrating superior areal capacitances (77.2 mF cm?2) and high energy density (3.86 μWh cm?2 at 0.12 mW cm?2) together with high user safety.  相似文献   

13.
A mesocellular silica–carbon nanocomposite foam (MSCF) is designed for the immobilization and biosensing of proteins. The as‐prepared MSCF has a highly ordered mesostructure, good biocompatibility, favorable conductivity and hydrophilicity, large surface area, and a narrow pore‐size distribution, as verified by transmission electron microscopy (TEM), IR spectroscopy, electrochemical impedance spectroscopy (EIS), nitrogen adsorption–desorption isotherms, pore size distribution plots, and water contact angle measurements. Using glucose oxidase (GOD) as a model, the MSCF is tested for immobilization of redox proteins and the design of electrochemical biosensors. GOD molecules immobilized in the mesopores of the MSCF show direct electrochemistry with a fast electron transfer rate (14.0 ± 1.7 s–1) and good electrochemical performance. Based on a decrease of the electrocatalytic response of the reduced form of GOD to dissolved oxygen, the proposed biosensor exhibits a linear response to glucose concentrations ranging from 50 μM to 5.0 mM with a detection limit of 34 μM at an applied potential of –0.4 V. The biosensor shows good stability and selectivity and is able to exclude interference from ascorbic acid (AA) and uric acid (UA) species that always coexist with glucose in real samples. The nanocomposite foam provides a good matrix for protein immobilization and biosensor preparation.  相似文献   

14.
“Regioselectivity deposition” method is developed to pattern silver electrodes facilely and efficiently by solution‐process with high resolution (down to 2 μm) on different substrates in A4 paper size. With the help of this method, large‐area, flexible, high‐performance polymer field‐effect transistors based on the silver electrodes and polyimide insulator are fabricated with bottom‐contact configuration by all‐solution processes. The polymer devices exhibit high performance with average field‐effect mobility over 1.0 cm2 V?1 s?1 (the highest mobility up to 1.5 cm2 V?1 s?1) and excellent environmental stability and flexibility, indicating the cost effectiveness of this method for practical applications in organic electronics.  相似文献   

15.
Assembling complex nanostructures on functional substrates such as electrodes promises new multi‐functional interfaces with synergetic properties capable of integration into larger‐scale devices. Here, we report a microemulsion‐mediated process for the preparation of CuO/Cu electrodes comprising a surface layer of a densely packed array of unusual cog‐shaped CuO microparticles with hierarchical nanofilament‐based superstructure and enhanced electrochemical performance in lithium‐ion batteries. The CuO particles are produced by thermolysis of Cu(OH)2 micro‐cog precursors that spontaneously assemble on the copper substrate when the metal foil is treated with a reactive oil‐based microemulsion containing nanometer‐scale aqueous droplets. The formation of the hierarchical superstructure improves the coulombic efficiency, specific capacity, and cycling performance compared with anodes based on CuO nanorods or polymer‐blended commercial CuO/C black powders, and the values for the initial discharge capacity (1052 mA h g?1) and reversible capacity (810 m A h g?1) are higher than most copper oxide materials used in lithium‐ion batteries. The results indicate that a fabrication strategy based on self‐assembly within confined reaction media, rather than direct synthesis in bulk solution, offers a new approach to the design of electrode surface structures for potential development in a wide range of materials applications.  相似文献   

16.
The concept of using ion conducting membranes (50–150 μm thick) for gating low‐voltage (1 V) organic field‐effect transistors (OFETs) is attractive due to its low‐cost and large‐area manufacturing capabilities. Furthermore, the membranes can be tailor‐made to be ion conducting in any desired way or pattern. For the electrolyte gated OFETs in general, the key to low‐voltage operation is the electrolyte “insulator” (the membrane) that provides a high effective capacitance due to ionic polarization within the insulator. Hydrous ion conducting membranes are easy to process and readily available. However, the role of the water in combination with the polymeric semiconductor has not yet been fully clarified. In this work electrical and optical techniques are utilized to carefully monitor the electrolyte/semiconductor interface in an ion conducting membrane based OFET. The main findings are that 1) moisture plays a major part in the transistor operation and careful control of both the ambient atmosphere and the potential differences between the electrodes are required for stable and consistent device behavior, 2) the obtained maximum effective capacitance (5 μF cm?2) of the membrane suggests that the electric double layer is distributed over a broad region within the polyelectrolyte, and 3) electromodulation spectroscopy combined with current–voltage characteristics provide a method to determine the threshold gate voltage from an electrostatic field‐effect doping to a region of (irreversible) electrochemical perturbation of the polymeric semiconductor.  相似文献   

17.
A novel hierarchical nanotube array (NTA) with a massive layered top and discretely separated nanotubes in a core–shell structure, that is, nickel–cobalt metallic core and nickel–cobalt layered double hydroxide shell (Ni?Co@Ni?Co LDH), is grown on carbon fiber cloth (CFC) by template‐assisted electrodeposition for high‐performance supercapacitor application. The synthesized Ni?Co@Ni?Co LDH NTAs/CFC shows high capacitance of 2200 F g?1 at a current density of 5 A g?1, while 98.8% of its initial capacitance is retained after 5000 cycles. When the current density is increased from 1 to 20 A g?1, the capacitance loss is less than 20%, demonstrating excellent rate capability. A highly flexible all‐solid‐state battery‐type supercapacitor is successfully fabricated with Ni?Co LDH NTAs/CFC as the positive electrode and electrospun carbon fibers/CFC as the negative electrode, showing a maximum specific capacitance of 319 F g?1, a high energy density of 100 W h kg?1 at 1.5 kW kg?1, and good cycling stability (98.6% after 3000 cycles). These fascinating electrochemical properties are resulted from the novel structure of electrode materials and synergistic contributions from the two electrodes, showing great potential for energy storage applications.  相似文献   

18.
We demonstrate 10 Gbps optical signal transmission via long‐range surface plasmon polaritons (LR‐SPPs) in a very thin metal strip‐guided geometry. The LR‐SPP waveguide was fabricated as a 14 nm thick, 2.5 μm wide, and 4 cm long gold strip embedded in a polymer and pigtailed with single‐mode fibers. The total insertion loss of 16 dB was achieved at a wavelength of 1.55 μm as a carrier wave. In a 10 Gbps optical signal transmission experiment, the LR‐SPP waveguide exhibits an excellent eye opening and a 2.2 dB power penalty at 10?12 bit error rate. We confirm, for the first time, that LR‐SPPs can efficiently transfer data signals as well as the carrier light.  相似文献   

19.
Potassium‐ion hybrid capacitors (PIHCs) show great potential in large‐scale energy storage due to the advantages of electrochemical capacitors and potassium‐ion batteries. However, their development remains at the preliminary stage and is mainly limited by the kinetic imbalance between the two electrodes. Herein, an architecture of NbSe2 nanosheets embedded in N, Se co‐doped carbon nanofibers (NbSe2/NSeCNFs) as flexible, free‐standing, and binder‐free anodes for PIHCs is reported. The NbSe2/NSeCNFs with hierarchically porous structure and N, Se co‐doping afford highly efficient channels for fast transportation of potassium ions and electrons during repeated cycling process. Furthermore, excellent electrochemical reversibility of the NbSe2/NSeCNFs electrode is demonstrated through in situ XRD, in situ Raman, ex situ transmission electron microscopy and element mapping. Thus, PIHCs with the NbSe2/NSeCNFs anode and active carbon cathode achieve a high energy of 145 W h kg?1 at a current density of 50 mA g?1, as well as an ultra‐long cycle life of over 10 000 cycles at a high current density of 2 A g?1. These results indicate that the assembled PIHCs display great potential for applications in the field of ultra‐long cycling energy storage devices.  相似文献   

20.
Novel composites of iron oxide encapsulated in macroporous silica with excellent arsenic adsorption performance have been successfully developed. Macroporous silica foams with large pore sizes of ≈100 nm and a high pore volume of 1.6 cm3 g?1 are chosen as the porous matrix. Electron tomography technique confirms that γ‐Fe2O3 nanoparticles with an average particle size of ≈6 nm are spatially well‐dispersed and anchored on the pore walls at even a high γ‐Fe2O3 content of 34.8 wt%, rather than forming aggregates inside the pores or on the external surface. The open large‐pore structure, high loading amount, and the non‐aggregated nature of γ‐Fe2O3 nanoparticles lead to increased adsorption sites and thus high adsorption capacities of both As (V) and As (III) without pre‐treatment (248 and 320 mg g?1, respectively). Moreover, the composites can reduce the concentration of both As (V) and As (III) from 100 to 2 μg L?1. It is also demonstrated that the composites can be applied in a household drinking water treatment device, which can continuously treat 20 L of wastewater containing As (V) with the effluent concentration lower than the World Health Organization standard.  相似文献   

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