Tannic acid-accelerated fenton chemical reaction amplification for fluorescent biosensing: The proof-of-concept towards ultrasensitive detection of DNA methylation.

As a promising biomarker, the level of methylated DNA usually changes in the early stage of the cancer. Ultrasensitive detection of the changes of methylated DNA offers possibility for early diagnosis of cancer. In this work, a tannic acid-accelerated Fenton chemical reaction amplification was firstly proposed for the construction of ultrasensitive fluorescent assay. Tannic acid was used as reductant to accelerate Fenton reaction procedure through the conversion of Fe3+/Fe2+, generating hydroxyl radicals (·OH) continuously. The produced ·OH oxidized massive non-fluorescent terephthalic acid (TA) to fluorescent-emitting hydroxy terephthalic acid (TAOH). In this way, the fluorescent signal could be greatly enhanced and the sensitivity was improved almost 116 times. The proposed signal amplification strategy was further applied to detect of DNA methylation with the assistance of liposome encapsulated with tannic-Fe3+ complexes. The methylated DNA was firstly captured through the hybridization with its complementary DNA that were pre-modified in the 96-well plate via the combination between streptavidin (SA) and biotin. Then, 5 mC antibody on the surface of liposomes specially recognized and combined with methylation sites, which brought large amount of tannic-Fe3+ complexes to participate Fenton reaction. The fluorescence of generated TAOH was depended on the concentration of methylated DNA. The assay showed good analytical performance for methylated DNA with a limit of detection (LOD) of 1.4 fM. It's believed that tannic acid-accelerated Fenton chemical reaction amplification strategy provides a promising platform for ultrasensitive fluorescent detection of low abundant biomarkers.

A Fluorescence Turn On-off-on Method for Sensitive Detection of Sn2+ and Glycine Using Waste Eggshell Membrane Derived Carbon Nanodots as Probe.

Changes in Sn2+ and glycine levels are relevant to many important physiological procedures in human health. However, investigation of their physiological functions is limited because few versatile methods towards Sn2+ and glycine detection have been developed. In this work, a fluorescence turn on-off-on strategy was firstly constructed for rapid and sensitive detection of Sn2+ and glycine through the specific binding between Sn2+ and glycine. Carbon nanodots (CDs) with a quantum yield of 19.5% were synthesized by utilizing inner film of waste eggshell as carbon source and employed as fluorescent probe. In the presence of Sn2+, the fluorescence of CDs was quenched by Sn2+ via the primary inner filter effect (IFE). However, the binding between Sn2+ and glycine prevented the IFE between Sn2+ and CDs, resulting in fluorescence recovery of CDs. Under optimized conditions, the fluorescent response of CDs displayed good linear relationships with the concentrations of Sn2+ in the range of 10-200 µM and 200-5000 µM, and the limit of detection (LOD) was 2.4 µM. For glycine detection, a good linear relationship was obtained in the concentration range of 5-1000 µM with a low LOD down to 0.76 µM. Moreover, the practicability of the assay was also demonstrated by measuring glycine content in human serum samples. This work provides an economical, green and fast method for biological analysis of Sn2+ and glycine.

In-situ formation of MnO2 nanoparticles on Ru@SiO2 nanospheres as a fluorescent probe for sensitive and rapid detection of glutathione.

Glutathione (GSH)-switched fluorescent assays have appealed much attention due to rapid signal changes of fluorescent probes. However, exposure to exterior environment of fluorescent probe causes photobleaching and premature leakage, leading to low sensitivity and poor photostability. Herein, luminescent SiO2 nanoparticles encapsulated with Ru(bpy)32+ (Ru@SiO2) were designed and synthesized as fluorescent probe to construct a GSH-switched fluorescent assay. The encapsulation of Ru(bpy)32+ in the SiO2 nanoparticles could effectively prevent the leakage of Ru(bpy)32+ molecules, improving the photostability of probe. The fluorescence of Ru@SiO2 nanoparticles was quenched by coating MnO2 nanoparticles on Ru@SiO2 surface (Ru@SiO2@MnO2 nanocomposites) through an in situ growth approach, which reduced background of the assay. The MnO2 nanoparticles not only further inhibited the leakage of Ru(bpy)32+ molecules, but also could serve as a recognition unit of GSH. In the presence of GSH, the MnO2 nanoparticles on the surface of Ru@SiO2 nanoparticles were reduced to Mn2+, resulting the fluorescence recovery of Ru@SiO2 nanoparticles. Thus, a signal-on fluorescent strategy was constructed for GSH detection. The assay displayed good analytical performance for GSH detection with a low detection limit of 16.2 nM due to excellent fluorescence quenching ability of MnO2 nanoparticles and special role of Ru@SiO2 nanoparticles to block probe leakage. The proposed assay was also applied to measure GSH levels in human serum samples. This work paves a new way to detect GSH with high sensitivity.

Interlayer-expanded VS2 nanosheet: Fast ion transport, dynamic mechanism and application in Zn2+ and Mg2+/Li+ hybrid batteries systems.

Currently, the development of polyvalent ions battery systems are still restricted by lacking suitable cathode materials with high energy density and long cycle life attributing to sluggish kinetic mechanism and of polyvalent ions. Herein, an effective inter-layer scaling strategy is proposed by using a simple hydrothermal method. The super layer spacing VS2 (∼1 nm) cathode dramatically improves electrochemical performance of zinc-ion batteries (ZIBs) and magnesium/lithium hybrid ion batteries (MLIBs). The specific discharge capacities of ZIBs and MLIBs are 450.7 and 488.8 mA h g-1 at current density of 0.1 A g-1 which are much higher than the same type of battery systems. Finally, the diffusion mechanism and the corresponding theoretical model is established by adopting first principles. In brief, the work provides an effective strategy for the large scale application of multivalent and hybrid batteries systems.

Dandelion-like CuCo2O4 arrays on Ni foam as advanced positive electrode material for high-performance hybrid supercapacitors.

In this paper, CuCo2O4 dandelion arrays grown on nickel foam (CuCo2O4/NF) was successfully synthesized by a simple hydrothermal route with post-heat-treatment for emolying as a high-performance positive electrode material for hybrid supercapacitors. Due to the unique tree-dimension porous (3D) microstructure and binder-free electrode architecture, the CuCo2O4/NF electrode deliveries a large specific capacitance of 2656.7 F g-1 at an areal current density of 1 mA cm-2. Moreover, it has an outstanding rate performance, as well as striking cycling stability. Additionally, a hybrid supercapacitors (HSCs) was fabricated using CuCo2O4 as positive electrode and corals-like N-doping porous carbon (N-CCs) as negative electrode. The device exhibited a broad potential window of 1.55 V and a high specific capacitance of 273.9 F g-1, which result in a largest energy density of 91.4 Wh kg-1 and a maximum power density of 13.4 kW kg-1. Finally, the assembled device manifests a preeminent electrochemical stability which maintained a 92.32% capacitance retention after 5000 cycles. The practical application was visually validated by lighting a blue light-emitting diode.

Three-dimensional flower-like MoS2-CoSe2 heterostructure for high performance superccapacitors.

A novel three-dimensional (3D) flower-like MoS2-CoSe2 heterostructure has been designed and synthesized by a facile two-step hydrothermal process as the electrode materials for supercapacitors. The MoS2-CoSe2 heterostructure is demonstrated to deliver a high specific capacitance (2577 F g-1 at 1 A g-1) and remarkable rate capability (896 F g-1 at 20 A g-1). Besides, the MoS2-CoSe2 electrode also exhibits excellent cycling stability of 91.03% capacitance retention after 5000 cycles even at a relatively high current density of 20 A g-1. A two-electrode configuration symmetric supercapacitor based MoS2-CoSe2 heterostructure delivers a maximum energy density of 60.5 W h kg-1 at a power density of 800 W kg-1 and the energy density remains at 35.6 W h kg-1 at a power density of 8000 W kg-1. Excellent cycling stability is also achieved with 83.62% retention after 2000 charge-discharge cycles, revealing its potential and viability for practical applications. The outstanding electrochemical performances of the fabricated electrode stem from the unique structure characteristic of the flower-like MoS2-CoSe2 heterostructure. The high-quality heterointerface facilitates electron conduction while the porosity not only allows fast ion transport but provides abundant active sites for Faradic reaction and the buffer for volume variety in repeat charge-discharge process. The design strategy offers a new idea for fabricating high-performance supercapacitor electrode materials.

Ultrasensitive electrochemical sensing platform based on graphene wrapping SnO2 nanocorals and autonomous cascade DNA duplication strategy.

In this work, a sensitive, universal and reusable electrochemical biosensor based on stannic oxide nanocorals-graphene hybrids (SnO2 NCs-Gr) is developed for target DNA detection by using two kinds of DNA enzymes for signal amplification through an autonomous cascade DNA duplication strategy. A hairpin probe is designed composing of a projecting part at the 3'-end as identification sequence for target, a recognition site for nicking endonuclease, and an 18-carbon shim to stop polymerization process. The designed DNA duplication-incision-replacement process is handled by KF polymerase and endonuclease, then combining with gold nanoparticles as signal carrier for further signal amplification. In the detection system, the electrochemical-chemical-chemical procedure, which uses ferrocene methanol, tris(2-carboxyethyl)phosphine and l-ascorbic acid 2-phosphate as oxidoreduction neurogen, deoxidizer and zymolyte, separately, is applied to amplify detection signal. Benefiting from the multiple signal amplification mechanism, the proposed sensor reveals a good linear connection between the peak current and logarithm of analyte concentration in range of 0.0001-1 × 10-11molL-1 with a detection limit of 1.25 × 10-17molL-1 (S/N=3). This assay also opens one promising strategy for ultrasensitive determination of other biological molecules for bioanalysis and biomedicine diagnostics.

Flower-like MoS2 decorated with Cu2O nanoparticles for non-enzymatic amperometric sensing of glucose.

In this study, a novel nanohybrid consisting of flower-like MoS2 decorated with Cu2O nanoparticles has been successfully synthesized for non-enzymatic amperometric sensing of glucose. Structural characterizations revealed that Cu2O nanoparticles were highly dispersed on MoS2 nanosheets. Electrochemical performances were investigated by cyclic voltammetry (CV) and chronoamperometry. Compared to single Cu2O component, the-synthesized Cu2O/MoS2 nanohybrid showed superior electrocatalysis to the oxidation of glucose. The fabricated non-enzymatic amperometric glucose sensor exhibited a wide linear range from 0.01 to 4.0mM with a low detection limit of 1.0µM (S/N =3) and a high sensitivity of 3108.87µAmM-1cm-2. Meanwhile, the non-enzymatic sensor also possesses satisfactory stability, good reproducibility and high selectivity to interfering components of uric acid, dopamine and ascorbic acid. The excellent analytical performances are resulted from the synergistic effect provided by the Cu2O nanoparticals and MoS2 nanosheets.

Au nanoparticles/hollow molybdenum disulfide microcubes based biosensor for microRNA-21 detection coupled with duplex-specific nuclease and enzyme signal amplification.

An ultrasensitive electrochemical biosensor for detecting microRNAs is fabricated based on hollow molybdenum disulfide (MoS2) microcubes. Duplex-specific nuclease, enzyme and electrochemical-chemical-chemical redox cycling are used for signal amplification. Hollow MoS2 microcubes constructed by ultrathin nanosheets are synthesized by a facile template-assisted strategy and used as supporting substrate. For biosensor assembling, biotinylated ssDNA capture probes are first immobilized on Au nanoparticles (AuNPs)/MoS2 modified electrode in order to combine with streptavidin-conjugated alkaline phosphatase (SA-ALP). When capture probes hybridize with miRNAs, duplex-specific nuclease cleaves the formative duplexes. At the moment, the biotin group strips from the electrode surface and SA-ALP is incapacitated to attach onto electrode. Then, ascorbic acids induce the electrochemical-chemical-chemical redox cycling to produce electrochemical response in the presence of ferrocene methanol and tris (2-carboxyethyl) phosphine. Under optimum conditions, the proposed biosensor shows a good linear relationship between the current variation and logarithm of the microRNAs concentration ranging from 0.1fM to 0.1pM with a detection limit of 0.086fM (S/N=3). Furthermore, the biosensor is successfully applied to detect target miRNA-21 in human serum samples.

Preparation of layered graphene and tungsten oxide hybrids for enhanced performance supercapacitors.

Tungsten oxide (WO3), which was originally poor in capacitive performance, is made into an excellent electrode material for supercapacitors by dispersing it on graphene (Gr). The obtained Gr-WO3 hybrids are characterized by X-ray diffraction, Raman spectroscopy, high-resolution transmission electron microscopy and scanning electron microscopy techniques, and evaluated as electrode materials for high-performance supercapacitors by cyclic voltammetry, galvanostatic charge-discharge curves and electrochemical impedance spectroscopy. A great improvement in specific capacitance is achieved with the present hybrids, from 255 F g-1 for WO3 nanoparticles to 580 F g-1 for Gr-WO3 hybrids (scanned at 1 A g-1 in 2 M KOH over a potential window of 0 to 0.45 V). The Gr-WO3 hybrid exhibits an excellent high rate capability and good cycling stability with more than 92% capacitance retention over 1000 cycles at a current density of 5 A g-1. The enhancement in supercapacitor performance of Gr-WO3 is not only attributed to its unique nanostructure with large specific surface area, but also its excellent electro-conductivity, which facilitates efficient charge transport and promotes electrolyte diffusion. As a whole, this work indicates that Gr-WO3 hybrids are a promising electrode material for high-performance supercapacitors.

Novel electrochemical dual-aptamer-based sandwich biosensor using molybdenum disulfide/carbon aerogel composites and Au nanoparticles for signal amplification.

A new electrochemical aptamer biosensor for the platelet-derived growth factor BB (PDGF-BB) detection has been developed based on the signal amplification of MoS2/carbon aerogel composites (MoS2/CA) and sandwich assay. A facile hydrothermal route assisted by L-cysteine was applied to synthesize CA incorporated flower-like MoS2 with the large surface active sites and good conductivity. The electrochemical aptasensor was constructed by sandwiching the PDGF-BB between a glassy carbon electrode modified with thiol-terminated PDGF-BB aptamer-1 (Apt1)/gold nanoparticles (AuNPs)/MoS2/CA and the AuNPs with thiol-terminated PDGF-BB aptamer-2 (Apt2) and 6-ferrocenyl hexanethiol (Fc). Fc-AuNPs-Apt2 acted as tracer and AuNPs/MoS2/CA were utilized as the biosensor platform to immobilize a large amount of capture aptamers, owing to their layered structure and high surface-to-volume ratio. Based on the sandwich format, a dual signal amplification strategy had been successfully developed with a wide linear response in the range of 0.001-10nM and a limit of detection of 0.3 pM. The developed assay demonstrated good selectivity and high sensitivity, indicating potential applications in bioanalysis and biomedicine.