Jing Lei

Hemin-functionalized MoS2 nanosheets: enhanced peroxidase-like catalytic activity with a steady state in aqueous solution

Hemin-functionalized MoS2 nanosheets (hemin/MoS2-NSs) are first obtained via van der Waals interactions between few-layered MoS2 nanosheets (MoS2-NSs) and hemin molecules. It is demonstrated that a portion of MoS2-NSs undergoes a phase transition from semiconducting to metallic phase under the influence of hemin, which shows the coexistence of semiconducting and metallic phases in the crystal structure of hemin/MoS2-NSs. MoS2-NSs prepared from sonication-induced exfoliation of bulk MoS2 crystals in aqueous surfactant solution exhibit intrinsic peroxidase-like activity for the oxidation of 3,3,5,5-tetramethylbenzidine in the presence of H2O2, which is further improved by the functionalization of hemin. Significantly, MoS2-NSs are presented as a new support of hemin, and when compared to MoS2-NSs, hemin/MoS2-NSs exhibit better dispersity in aqueous solution, which is used in the development of H2O2 sensor based on the enhanced peroxidase-like activity.

Highly selective and sensitive electrochemical biosensor for ATP based on the dual strategy integrating the cofactor-dependent enzymatic ligation reaction with self-cleaving DNAzyme-amplified electrochemical detection.

A dual strategy that combines the adenosine triphosphate (ATP)-dependent enzymatic ligation reaction with self-cleaving DNAzyme-amplified electrochemical detection is employed to construct the biosensor. In this design, the methylene blue-labeled hairpin-structured DNA was self-assembled onto a gold electrode surface to prepare the modified electrode through the interaction of Au-S bond. In the procedure of ATP-dependent ligation reaction, when the specific cofactor ATP was added, the two split oligonucleotide fragments of 8-17 DNAzyme were linked by T4 DNA ligase and then released to hybridize with the labeled hairpin-structured DNA substrate. The linked 8-17 DNAzyme catalyzes the cleavage of the hairpin-structured substrate by the addition of Zn(2+), causing the methylene blue which contains high electrochemical activity to leave the surface of the gold electrode, therefore generating a dramatic decrease of electrochemical signal. The decrease of peak current was readily measured by square wave voltammetry and a relatively low detection limit (0.05 nM) was obtained with a linear response range from 0.1 to 1000 nM. By taking advantage of the highly specific cofactor dependence of the DNA ligation reaction, the proposed ligation-induced DNAzyme cascades demonstrate ultrahigh selectivity toward the target cofactor ATP. A catalytic and molecular beacons strategy is further adopted to amplify the electrochemical signal detection achieved by cycling and regenerating the 8-17 DNAzyme to realize enzymatic multiple turnover, thus one DNAzyme can catalyze the cleavage of several hairpin-structured substrates, which improves the sensitivity of the newly designed electrochemical sensing system.

Water-Soluble Nonconjugated Polymer Nanoparticles with Strong Fluorescence Emission for Selective and Sensitive Detection of Nitro-Explosive Picric Acid in Aqueous Medium

Water-soluble nonconjugated polymer nanoparticles (PNPs) with strong fluorescence emission were prepared from hyperbranched poly(ethylenimine) (PEI) and d-glucose via Schiff base reaction and self-assembly in aqueous phase. Preparation of the PEI-d-glucose (PEI-G) PNPs was facile (one-pot reaction) and environmentally friendly under mild conditions. Also, PEI-G PNPs showed a high fluorescence quantum yield in aqueous solution, and the fluorescence properties (such as concentration- and solvent-dependent fluorescence) and origin of intrinsic fluorescence were investigated and discussed. PEI-G PNPs were then used to develop a fluorescent probe for fast, selective, and sensitive detection of nitro-explosive picric acid (PA) in aqueous medium, because the fluorescence can be easily quenched by PA whereas other nitro-explosives and structurally similar compounds only caused negligible quenching. A wide linear range (0.05-70 μM) and a low detection limit (26 nM) were obtained. The fluorescence quenching mechanism was carefully explored, and it was due to a combined effect of electron transfer, resonance energy transfer, and inner filter effect between PA and PEI-G PNPs, which resulted in good selectivity and sensitivity for PA. Finally, the developed sensor was successfully applied to detection of PA in environmental water samples.

A regenerative ratiometric electrochemical biosensor for selective detecting Hg2+ based on Y-shaped/hairpin DNA transformation

Inspired by dual-signaling ratiometric mechanism which could reduce the influence of the environmental change, a novel, convenient, and reliable method for the detection of mercury ions (Hg(2+)) based on Y-shaped DNA (Y-DNA) was developed. Firstly, the Y-DNA was formed via the simple annealing way of using two different redox probes simultaneously, omitting the multiple operation steps on the electrode. The Y-DNA was immobilized on the gold electrode surface and then an obvious ferrocene (Fc) signal and a weak methylene blue (MB) signal were observed. Upon addition of Hg(2+), the Y-DNA structure was transformed to hairpin structure based on the formation of T-Hg(2+)-T complex. During the transformation, the redox MB gets close to and the redox Fc gets far away from the electrode surface, respectively. This special design allows a reliable Hg(2+) detection with a detection range from 1 nM to 5 μM and a low detection limit down to 0.094 nM. Furthermore, this biosensor exhibits good selectivity and repeatability, and can be easily regenerated by using L-cysteine. This study offers a simple and effective method for designing ratiometric biosensors for detecting other ions and biomolecules.

Application of a cosmetic additive as an eco-friendly inhibitor for mild steel corrosion in HCl solution

The use of the cosmetic ingredient cocamidopropylamine oxide (CAO) to inhibit the corrosion of steel in 0.5mol/LHCl is investigated. Electrochemical and weight loss methods were used to evaluate the inhibiting effect of CAO and the influences of inhibitor concentration and temperature were determined. It was found that CAO acted as a mix-type inhibitor and was adsorbed chemically onto the steel in HCl solution, and the maximum inhibition efficiency was found at critical micelle concentration (CMC) of CAO in tested corrosive media. Moreover, it was speculated that relationships of the two adsorption sites of the inhibitor and steel surface were different.

Diverse States and Properties of Polymer Nanoparticles and Gel Formed by Polyethyleneimine and Aldehydes and Analytical Applications

Multicolor polymer nanoparticles (or dots) were prepared via the reaction between hyperbranched polyethyleneimine (PEI) and aldehydes, and when the concentration of aldehydes was lower, the final mixture displayed gelation behavior. This phenomenon can be applied to visual detection of aldehydes. Moreover, the colors of the polymer dots and gel are varied by using different kinds of aldehydes, which can be utilized for visual discrimination of aldehydes. For simplicity, we focus our attention on the interaction between PEI and formaldehyde. The nanoparticles show an average diameter of 42 nm, emit bright cyan fluorescence with high quantum yield, and exhibit high water dispersibility and excellent photostability. Due to the advantages, our polymer nanoparticles (PNPs) are utilized as a fluorescent probe for imaging in living SK-N-SH cells. Furthermore, valuable explorations have been carried out on the fundamental properties of PNPs, such as concentration-dependent fluorescence, pH-dependent fluorescence, and solvent effect.

An electrochemical sensor for sodium dodecyl sulfate detection based on anion exchange using eosin Y/polyethyleneimine modified electrode

A simple and effective method for the detection of electrochemically inactive sodium dodecyl sulfate (SDS) has been designed, based on different binding affinity of polyethyleneimine (PEI) toward electrochemically active eosin Y and electrochemically inactive SDS. The stronger binding affinity of the PEI toward SDS than eosin Y results in the decrease of the redox peak current of surface confined eosin Y and provides a quantitative readout for the SDS. The difference in value of the cathodic peak current showed a linear relationship with SDS concentration in a concentration range from 1 to 40 μg mL(-1), and a detection limit of 0.9 μg mL(-1) for SDS was obtained. Furthermore, the method has been successfully applied to the detection of SDS in real samples. The developed approach provided a simple and reliable detection for SDS and might have potential applications in electrochemical methods for inactive molecules.

A regenerative electrochemical biosensor for mercury(II) by using the insertion approach and dual-hairpin-based amplification.

A simple and effective biosensor for Hg(2+) determination was investigated. The novel biosensor was prepared by the insertion approach that the moiety-labeled DNA inserted into a loosely packed cyclic-dithiothreitol (DTT) monolayer, improving the hybridization efficiency. Electrochemical impedance spectroscopy studies of two biosensors (single-hairpin and dual-hairpin structure DNA modified electrodes) used for Hg(2+) detection indicated that the dual-hairpin modified electrode had a larger electron transfer resistance change (ΔRct). Consequently, the dual-hairpin structure was used as a signal amplifier for the preparation of a selective Hg(2+) biosensor. This biosensor exhibited an excellent selectivity toward Hg(2+) over Cd(2+), Pd(2+), Co(2+) etc. Also, a linear relation was observed between the ΔRct and Hg(2+) concentrations in a range from 0.1 nM to 5 μM with a detection limit of 28 pM under optimum conditions. Moreover, the biosensor can be reused by using L-cysteine and successfully applied for detecting Hg(2+) in real samples.

A regenerated electrochemical biosensor for label-free detection of glucose and urea based on conformational switch of i-motif oligonucleotide probe

Improving the reproducibility of electrochemical signal remains a great challenge over the past decades. In this work, i-motif oligonucleotide probe-based electrochemical DNA (E-DNA) sensor is introduced for the first time as a regenerated sensing platform, which enhances the reproducibility of electrochemical signal, for label-free detection of glucose and urea. The addition of glucose or urea is able to activate glucose oxidase-catalyzed or urease-catalyzed reaction, inducing or destroying the formation of i-motif oligonucleotide probe. The conformational switch of oligonucleotide probe can be recorded by electrochemical impedance spectroscopy. Thus, the difference of electron transfer resistance is utilized for the quantitative determination of glucose and urea. We further demonstrate that the E-DNA sensor exhibits high selectivity, excellent stability, and remarkable regenerated ability. The human serum analysis indicates that this simple and regenerated strategy holds promising potential in future biosensing applications.