Liming Qi

Synthesis of Convex Hexoctahedral Palladium@Gold Core–Shell Nanocrystals with {431} High-Index Facets with Remarkable Electrochemiluminescence Activities

Convex hexoctahedral nanocrystals have been synthesized through fast growth kinetics and the use of cetylpyridinium chloride as a capping agent. Monodisperse convex hexoctahedral Pd@Au core-shell nanocrystals with {431} high-index facets are obtained at high reaction rates by using high concentrations of ascorbic acid in the presence of cetylpyridinium chloride. In contrast, octahedral nanocrystals with {111} low-index facets and their {100}-truncated counterparts are formed at low ascorbic acid concentrations. The substitute of cetylpyridinium chloride with cetyltrimethylammonium chloride leads to the generation of concave trisoctahedral Pd@Au core-shell nanocrystals with {331} high-index facets, indicating that cetylpyridinium plays an important role in the formation of convex hexoctahedral nanocrystals. The as-prepared convex hexoctahedral Pd@Au core-shell nanocrystals exhibit remarkable catalytic performances toward electrochemiluminescence compared with truncated octahedral and concave trisoctahedral Pd@Au core-shell nanocrystals.

Ultrasensitive Glutathione Detection Based on Lucigenin Cathodic Electrochemiluminescence in the Presence of MnO2 Nanosheets

Glutathione (GSH) is a crucial antioxidant produced endogenously and plays key roles in biological systems. It is vitally important to design simple, selective, and sensitive methods to sense GSH and monitor changes of GSH concentration. In this work, the cathodic electrochemiluminescence (ECL) of lucigenin in the presence of MnO2 nanosheets at a glassy carbon electrode was utilized for GSH detection. GSH can reduce MnO2 nanosheets into Mn(2+) which can obviously inhibit the ECL of lucigenin. The ECL inhibition efficiencies increase linearly with the concentrations of glutathione in the range of 10 to 2000 nM. The detection limit for GSH measurement is 3.7 nM. This proposed method is highly sensitive, selective, simple, fast, and cost-effective. Moreover, this approach can detect GSH in human serum samples with excellent recoveries, which indicates its promising application under physiological conditions.

Chemiluminescence of creatinine/H2O2/Co2+ and its application for selective creatinine detection

Creatinine is an important biomarker in clinical diagnosis and biomonitoring programs as well as urinary metabolomic/metabonomics research. Current methods are either nonselective, time consuming or require heavy and expensive instruments. In this study, chemiluminescence of creatinine with hydrogen peroxide has been reported for the first time, and its chemiluminescence is remarkably enhanced in the presence of cobalt ions. By utilizing these phenomena, we have developed a sensitive and selective chemiluminescence method for creatinine determination by coupling with flow injection analysis. The calibration curve is linear in the range of 1×10(-7)-3×10(-5)mol/L with a limit of detection (S/N=3) of 7.2×10(-8)mol/L, which is adequate for detecting creatinine in the clinically accepted range. The relative standard deviation for seven measurements of 3×10(-5)mol/L creatinine is 1.2%. The chemiluminescence method was then utilized to detect creatinine in human urine samples after simple dilution with water. It takes less than 1min each measurement and the recoveries for spiked urine samples were 100-103%. The interference study demonstrates that some common species in urine, such as amino acids, ascorbic acid and creatine, have negligible effects on creatinine detection. The present method does not use expensive instruments, enzymes and separation technique. This method has the advantages of sensitivity, selectivity, simplicity, rapidity, and low cost. It holds great promise for basic or comprehensive metabolic panel, drug screening, anti-dopping, and urinary metabolomic/metabonomics research.

Stainless Steel Electrode for Sensitive Luminol Electrochemiluminescent Detection of H2O2, Glucose, and Glucose Oxidase Activity

Electrogenerated chemiluminescence (ECL) application of stainless steel, a robust and cost-effective material, has been developed for the first time. Type 304 stainless steel electrode shows appealing ECL performance in the luminol-H2O2 system. It enables the detection of H2O2 with a linear range from 1 to 1000 nM and a limit of detection of 0.456 nM [signal-to-noise ratio (S/N) = 3]. The ECL method based on type 304 stainless steel electrode is more sensitive, more cost-effective, and much simpler than other ECL methods reported before. Because the stainless steel electrode has excellent performance for H2O2 detection and H2O2 participates in many important enzymatic reactions, applications of stainless steel electrode-based ECL for detection of enzyme activities and enzyme substrates were further investigated by use of glucose oxidase (GODx) and glucose as representative enzyme and substrate. The concentrations of glucose and the activity of GODx were directly proportional to ECL intensities over a range of 0.1-1000 μM and 0.001-0.7 units/mL with limits of detection of 0.076 μM and 0.00087 unit/mL (S/N = 3), respectively. This method was successfully used for determining glucose in honey. Because of their remarkable performance and user-friendly features, stainless steel electrodes hold great promise in various electroanalytical applications, such as biosensing, disposable sensors, and wearable sensors.

Increasing Electrochemiluminescence Intensity of a Wireless Electrode Array Chip by Thousands of Times Using a Diode for Sensitive Visual Detection by a Digital Camera.

Both a wireless electrochemiluminescence (ECL) electrode microarray chip and the dramatic increase in ECL by embedding a diode in an electromagnetic receiver coil have been first reported. The newly designed device consists of a chip and a transmitter. The chip has an electromagnetic receiver coil, a mini-diode, and a gold electrode array. The mini-diode can rectify alternating current into direct current and thus enhance ECL intensities by 18 thousand times, enabling a sensitive visual detection using common cameras or smart phones as low cost detectors. The detection limit of hydrogen peroxide using a digital camera is comparable to that using photomultiplier tube (PMT)-based detectors. Coupled with a PMT-based detector, the device can detect luminol with higher sensitivity with linear ranges from 10 nM to 1 mM. Because of the advantages including high sensitivity, high throughput, low cost, high portability, and simplicity, it is promising in point of care testing, drug screening, and high throughput analysis.

Chemiluminescence and electrochemiluminescence applications of metal nanoclusters

Due to strong photoluminescence, extraordinary photostability, excellent biocompatibility, and good water-solubility, metal nanoclusters have attracted enormous attention since discovered. They are found to be novel fluorescence labels for biological applications and environmental monitoring. Recently the chemiluminescence (CL) or electrochemiluminescence (ECL) of metal nanoclusters has received increasing attention. This review covers recent vibrant developments in this field of the past 5 years, and highlights different functions of metal nanoclusters in various CL and ECL systems, such as luminophores, catalysts, and quenchers. Latest synthetic methods of metal nanoclusters used in CL or ECL are also summarized. Furthermore, we discuss some perspectives and critical challenges of this field in the near future.

Development of luminol-N-hydroxyphthalimide chemiluminescence system for highly selective and sensitive detection of superoxide dismutase, uric acid and Co2+

N-hydroxyphthalimide (NHPI), a well known reagent in organic synthesis and biochemical applications, has been developed as a stable and efficient chemiluminescence coreactant for the first time. It reacts with luminol much faster than N-hydroxysuccinimide, eliminating the need of a prereaction coil used in N-hydroxysuccinimide system. Without using prereaction coil, the chemiluminescence peak intensities of luminol-NHPI system are about 102 and 26 times greater than that of luminol-N-hydroxysuccinimide system and classical luminol-hydrogen peroxide system, respectively. The luminol-NHPI system achieves the highly sensitive detection of luminol (LOD = 70pM) and NHPI (LOD = 910nM). Based on their excellent quenching efficiencies, superoxide dismutase and uric acid are sensitively detected with LODs of 3ng/mL and 10pM, respectively. Co2+ is also detected a LOD of 30pM by its remarkable enhancing effect. Noteworthily, our method is at least 4 orders of magnitude more sensitive than previously reported uric acid detection methods, and can detect uric acid in human urine and Co2+ in tap and lake water real samples with excellent recoveries in the range of 96.35-102.70%. This luminol-NHPI system can be an important candidate for biochemical, clinical and environmental analysis.

3D Printed Rotating Acentric Binary-disk Electrode

Rotating ring-disk electrode (RRDE) is a generator-collector electrochemical system widely used as an electroanalytical and kinetic device. However, RRDEs are costly and difficult to fabricate, particularly when the electrode material is fragile, small, and scarce. Taking advantage of readily available 3D printing technology an alternative generator-collector system was developed: rotating acentric binary-disk electrode (RABDE). RABDE consists of two close acentric disk electrodes arranged in a cylindrical matrix so that the line connecting their centers is perpendicular to radius of the device passing through the center of generator electrode. In contrast to RRDE that is based on radial flow velocity for mass transfer between the generator and the collector, RABDE mostly takes advantage of the larger tangential flow velocity. RABDE thus exhibits higher current densities than RRDE for a same rotation rate and evidences much better electroanalytical performances. These increased performances were tested and quantified using typical analytes: potassium ferricyanide system, copper ion system, and oxygen reduction reaction in alkaline solution.