Study on the Enhancement of Electrochemical and Electrochemiluminescence Behaviors of Au-Ag Nanoclusters Based on Synergistic and Ligand Effects.

A simultaneous electrochemical (EC) and electrochemiluminescence (ECL) detection scheme was introduced to both microchip and conventional capillary electrophoresis (CE). In this dual detection scheme, tris(2,2'-bipyridyl)ruthenium(II) (Ru(bpy)3(2+)) was used as an ECL reagent as well as a catalyst (in the formation of Ru(bpy)3(3+)) for the EC detection. In the Ru(bpy)3(2+)-ECL process, Ru(bpy)3(3+) was generated and then reacted with analytes resulting in an ECL emission and a great current enhancement in EC detection due to the catalysis of Ru(bpy)3(3+). The current response and ECL signals were monitored simultaneously. In the experiments, dopamine and three kinds of pharmaceuticals, anisodamine, ofloxacin, and lidocaine, were selected to validate this dual detection strategy. Typically, for the EC detection of dopamine with the presence of Ru(bpy)3(2+), a approximately 5 times higher signal-to-noise ratio (S/N) can be achieved than that without Ru(bpy)3(2+), during the simultaneous EC and ECL detection of a mixture of dopamine and lidocaine using CE separation. The results indicated that this dual EC and ECL detection strategy could provide a simple and convenient detection method for analysis of more kinds of analytes in CE separation than the single EC or ECL detection alone, and more information of analytes could be achieved in analytical applications simultaneously.

Amphetamines including methamphetamine, 3,4-methylenedioxyamphetamine and 3,4-methylenedioxymethamphetamine were separated and detected by CE using simultaneous electrochemical (EC) and electrochemiluminescence (ECL) detection (CE-EC/ECL). Factors that influenced the separation and detection performance, such as the detection potential, the pH value and concentration of the running buffer, the separation voltage and the pH of the detection buffer, were investigated. LODs of 3.3x10(-8) mol/L (0.16 fmol), 1.6x10(-7) mol/L (0.78 fmol) and 3.3x10(-8) mol/L (0.16 fmol) were obtained for methamphetamine, 3,4-methylenedioxyamphetamine and 3,4-methylenedioxymethamphetamine, respectively. For practical application, a liquid-liquid extraction with ethyl acetate procedure was developed for urine sample pretreatment and extraction efficiencies higher than 90% were obtained. The established simultaneous CE-EC/ECL was successfully applied for urine sample analysis.

Recent advances and key strategies in capillary electrophoresis and microchip CE with electrochemical detection (ECD) and electrochemiluminescence (ECL) detection are reviewed. This article consists of four main parts: CE-ECD; microchip CE-ECD; CE-ECL; and microchip CE-ECL. It is expected that ECD and ECL will become powerful tools for CE microchip systems and will lead to the creation of truly disposable devices. The focus is on papers published in the last two years (from 2005 to 2006).

Bridging Au nanoclusters with ultrathin LDH nanosheets via ligands for enhanced charge transfer in photocatalytic CO2 reduction

Electrochemiluminescence (ECL) is a light-emitting process which combines the intriguing merits of both electrochemical and chemiluminescent methods. It is an extensively used method especially in clinical analysis and biological research due to its high sensitivity, wide dynamic range, and good reliability. ECL devices are critical for the development and applications of ECL. Much effort has been expended to improve the sensitivity, portability, affordability, and throughput of new ECL devices, which allow ECL to adapt broad usage scenarios.In this Account, we summarize our efforts on the recent development of ECL devices including new electrodes, ECL devices based on a wireless power transfer (WPT) technique, and novel bipolar electrochemistry. As the essential components in the ECL devices, electrodes play an important role in ECL detection. We have significantly improved the sensitivity of luminol ECL detection of H2O2 by using a stainless steel electrode. By using semiconductor materials (e.g., silicon and BiVO4), we have exploited photoinduced ECL to generate intense emission at much lower potentials upon illumination. For convenience, portability, and disposability, ECL devices based on cheap WPT devices have been designed. A small diode has been employed to rectify alternating current into direct current to dramatically enhance ECL intensity, enabling sensitive ECL detection using a smart phone as a detector. Finally, we have developed several ECL devices based on bipolar electrochemistry in view of the convenience of multiplex ECL sensing using a bipolar electrode (BPE). On the basis of the wireless feature of BPE, we have employed movable BPEs (e.g., BPE swimmers and magnetic rotating BPE) for deep exploration of the motional and ECL properties of dynamic BPE systems. To make full use of the ECL solution, we have dispersed numerous micro-/nano-BPEs in solution to produce intense 3D ECL in the entire solution, instead of 2D ECL in conventional ECL devices. In addition, the interference of ECL noise from driving electrodes was minimized by introducing the stainless steel with a passivation layer as the driving electrode. To eliminate the need for the fabrication of electrode arrays and the interference from the driving electrode and to decrease the applied voltage, we develop a new-type BPE device consisting of a single-electrode electrochemical system (SEES) based on a resistance-induced potential difference. The SEES is fabricated easily by attaching a multiperforated plate to a single film electrode. It enables the simultaneous detection of many samples and analytes using only a single film electrode (e.g., screen-printed electrode) instead of electrode arrays. It is of great potential in clinical analysis especially for multiple-biomarker detection, drug screening, and biological studies. Looking forward, we believe that more ECL devices and related ECL materials and detection methods will be developed for a wide range of applications, such as in vitro diagnosis, point-of-care testing, high-throughput analysis, drug screening, biological study, and mechanism investigation.

Microreactor and electrochemical detectors fabricated using Si and EPON SU-8

Kaiser score diagnosis of breast MRI lesions: Factors associated with false-negative and false-positive results

CE coupled with dual electrochemical (EC) and electrochemiluminescence (ECL) detection was optimized for simultaneous analysis of six cardiovascular drugs (alprenolol, propafenone, acebutolol, verapamil, atenolol and metoprolol) via central composite design. Following this study, three critical electrophoretic factors governing the CE separation were investigated: Tris-H(3)PO(4) buffer concentration, buffer pH value and separation voltage. A modified chromatographic response was adopted for evaluating CE separation quality. Optimum conditions were achieved using Tris-H(3)PO(4) buffer 35.6 mM (pH 2.3) separated at 13.9 kV, which was employed experimentally and led to the successful simultaneous separation of the above six drugs. The good agreement of the chromatographic response was observed between predicted data and actual experimental results using these optimized conditions (RSD=3.75%). The proposed method was validated for linearity, repeatability and sensitivity, and subsequently successfully applied to determine six basic drugs in urine samples.

Enhanced near-infrared electrochemiluminescence of Au nanoclusters treated with piperidine

The Lifetime Economic Burden of Inaccurate HER2 Testing: Estimating the Costs of False-Positive and False-Negative HER2 Test Results in US Patients with Early-Stage Breast Cancer

In this presentation, a unique generation of near-infrared electrochemiluminescence (ECL) from water-soluble Au nanoclusters is discussed. Specifically, we report the near-infrared ECL of glutathione-stabilized Au nanoclusters, of which the photoluminescence is primarily within the visible wavelength region. Detailed experimental studies, including spooling ECL spectroscopy and time-resolved optical measurements, suggested that the near-infrared ECL is ascribed to the Au(0)-glutathione motif in the Au nanoclusters. Further studies of individual Au nanoclusters fractionated by gel electrophoresis of as-synthesized Au nanoclusters also revealed that the individual Au nanoclusters exhibited near-infrared ECL that became dominant when the ratio of Au(0) to Au(I) increased in the individual nanoclusters. These indicated that the oxidation states of Au nanoclusters primarily affected the ECL wavelengths of the nanoclusters because the Au(0)-glutathione motif in the nanoclusters was responsible for the near-infrared ECL emission.

Risk of false compliance/non-compliance decisions for sterility test due to false-negative and false-positive test results

Portable electrochemiluminescence detection system based on silicon photomultiplier single photon detector and aptasensor for the detection of tetracycline in milk

The electrochemical and electrochemiluminescence (ECL) detection of cell lines of Burkitt's lymphoma (Ramos) by using magnetic beads as the separation tool and high-affinity DNA aptamers for signal recognition is reported. Au nanoparticles (NPs) bifunctionalized with aptamers and CdS NPs were used for electrochemical signal amplification. The anodic stripping voltammetry technology employed for the analysis of cadmium ions dissolved from CdS NPs on the aggregates provided a means to quantify the amount of the target cells. This electrochemical method could respond down to 67 cancer cells per mL with a linear calibration range from 1.0×10(2) to 1.0×10(5) cells mL(-1), which shows very high sensitivity. In addition, the assay was able to differentiate between target and control cells based on the aptamer used in the assay, indicating the wide applicability of the assay for diseased cell detection. ECL detection was also performed by functionalizing the signal DNA, which was complementary to the aptamer of the Ramos cells, with tris(2,2-bipyridyl) ruthenium. The ECL intensity of the signal DNA, replaced by the target cells from the ECL probes, directly reflected the quantity of the amount of the cells. With the use of the developed ECL probe, a limit of detection as low as 89 Ramos cells per mL could be achieved. The proposed methods based on electrochemical and ECL should have wide applications in the diagnosis of cancers due to their high sensitivity, simplicity, and low cost.

Electrochemiluminescence and electrochemical dual-mode detection of BACE1 activity based on the assembly of peptide and luminol co-functionalized silver nanoparticles induced by cucurbit[8]uril