Latest ArticlesHerein, we propose a novel photoelectrochemical (PEC) biosensor for dual microRNAs (miRNAs) highly sensitive and simultaneous biosensing based on strand displaced amplification (SDA) reaction. The recognition of HmiR-21 and Hlet-7a by microRNA-21 and let-7a leads to their change in hairpin structures, subsequently initiating the immobilization of abundant CdS quantum dots (CdS QDs) and methylene blue (MB) based on SDA reaction. The immobilized CdS QDs and MB produce both high PEC currents under 430 nm light and 627 nm light illumination, respectively, and the generated PEC currents are closely relied on target miRNAs amounts. Thus, highly sensitive and simultaneous detection of microRNA-21 Herein, we propose a novel photoelectrochemical (PEC) biosensor for dual microRNAs (miRNAs) highly sensitive and simultaneous biosensing based on strand displaced amplification (SDA) reaction. The recognition of HmiR-21 and Hlet-7a by microRNA-21 and let-7a leads to their change in hairpin structures, subsequently initiating the immobilization of abundant CdS quantum dots (CdS QDs) and methylene blue (MB) based on SDA reaction. The immobilized CdS QDs and MB produce both high PEC currents under 430 nm light and 627 nm light illumination, respectively, and the generated PEC currents are closely relied on target miRNAs amounts. Thus, highly sensitive and simultaneous detection of microRNA-21 and let-7a was readily achieved with detection limit at 6.6 fmol/L and 15.4 fmol/L based on 3σ, respectively. Further, this PEC biosensor was applied in simultaneous analysis of miRNA-21 and let-7a in breast cancer patient's serum with acceptable results. We expect this biosensor will find more useful application in diagnosis of miRNA-related diseases.
Transition-metal chalcogenides with hollow nanostructure, especially cobalt sulfides, are considered as the most promising non-precious metal catalysts for oxygen evolution reaction. However, it is difficult to synthesize oxygen-containing cobalt sulphides with hollow structure due to the different physical/chemical properties between metal sulfides and metal cobalts. Herein, we report a novel oxygen-containing amorphous cobalt sulfide ball-in-ball hollow spheres (Co-S-O BBHS) synthesized by an anion exchange method. Taking advantage of the ball-in-ball hollow structure, the amorphous Co-S-O BBHS shows superior oxygen evolution reaction (OER) electrocatalytic performance with a low overpotential of 285 mV at 10 mA/cm2, small Tafel slope of 49.67 mV/dec, high Faraday efficiency of 96%, and satisfied durability. Experiments and DFT calculations demonstrate that the introduction of oxygen and sulfur modulates the electronic structure of Co-S-O BBHS, thus enhancing the adsorption of *O (adsorbed O species on catalyst surface) intermediate, which greatly boosts the catalytic activity towards OER. This work provides a new strategy for controllable synthesis of complex hollow structures of transition-metal chalcogenides for OER.
Metal-free heteroatoms dual-doped carbon has been recognized as one of the most promising Pt/C-substitutes for oxygen reduction reaction (ORR). Herein, we optimize the preparation process by doping order of metal-free heteroatoms to obtain the best electrocatalytic performance through three types of dual-doped carbon, including XC-N (first X doping then N doping), NC-X (first N doping then X doping) and NXC (N and X doping) (X = P, S and F). XC-N has more defect than the other two indicated by Raman spectra. X-ray photoelectron spectrom (XPS) measurements indicate that N and X have been dual-doped into the carbon matrix with different doping contents and modes. Electrocatalytic results, including the potential of ORR peak (Ep), the half-wave potential, the diffusion-limiting current density mainly follows the order of XC-N > NC-X > NXC. Furthermore, the synergistic effect of second atom doping are also compared with the single doped carbon (NC, PC, SC and FC). The differences in electronegativity and atomic radius of these metal-free heteroatoms can affect the defect degree, the doping content and mode of heteroatoms on carbon matrix, induce polarization effect and space effect to affect O2 adsorption and product desorption, ultimately to the ORR electrocatalytic performance.
CeO2 morphology was proposed to be a crucial factor for reducing nitrobenzene to azoxybenzene under the base-free condition. Herein, the structure-activity relationship of CeO2 catalysts was explored to improve the azoxybenzene yield. A series of CeO2 catalysts were synthesized with seven morphologies to obtain different Ce3+ proportion and various surface areas. Notably, the catalytic performance of these samples for reducing nitrobenzene to azoxybenzene enhanced with the increasing Ce3+ proportion. With the highest surface Ce3+ proportion, the Rod-CeO2 catalyst exhibited 100% conversion of nitrobenzene and 89.8% azoxybenzene selectivity in 7 h at 150 ℃ under 1 MPa CO. Moreover, the preliminary mechanistic analysis indicated that the inhabitation of azoxybenzene to by-product azobenzene resulted in the high selectivity of azoxybenzene.
Ion diffusion kinetics, depending on the size, tortuosity, connectivity of the channels, greatly affects the rate performance of the electrodes. Two-dimensional materials (2DMs) has emerged as promising electrode materials in the past decades. However, the applications of 2DMs electrodes are limited by the strong restacking problem, which leads to a poor rate capability. In this work, we for the first time mediated the morphology of molybdenum disulfide (MoS2) nanosheets via a facile coagulation method; abundant sheet crumples were induced, which greatly enhance their surface accessibility and thus benefit the ion diffusion kinetics. Consequently, the crumpled-MoS2 electrodes follow a capacitive Na-ion charge-storage mechanism to a large extent. Importantly, we demonstrate the special role of organic cations in the inter-sheet assembly configuration, in sharp contrast with that of alkali/alkaline-earth ones. We propose that organic cations cause edge/face contact of the sheets, instead of the face/face contact, thus affording a house-of-cards structure.
Light utilization is one of the key factors for the improvement of photocatalytic performance. Herein, we design C-TiO2 hollow nanoshells with strong Mie resonance for enhanced photocatalytic hydrogen evolution in a dye-sensitized system under visible light irradiation (λ≥420 nm). By tuning the inner diameters of hollow nanoshells, the Mie resonance in hollow nanoshells is adjusted for better excitation of dye molecules, which thus greatly enhances the light utilization in visible light region. This work shows the potential of Mie resonance in nanoshells can be an alternative strategy to increase the light utilization for photocatalysis.
A new family of isostructural 3d-4f polymetallic complexes, formulated as [Cu6Ln5(μ3−OH)9 (C4H8O2N)6(C5H4ON)6(H2O)9]·(ClO4)6·(H2O)22 (Ln = Pr, 1; Nd, 2; Sm, 3; Eu, 4; Gd, 5), was successfully isolated through the simple hydrolysis reaction of 2-aminoisobutyric acid, 2-hydroxypyridine, Cu(CH3COO)2·H2O, and Ln(ClO4)3·6H2O. Notably, the [Cu6Ln5] clusters with high molecular symmetry of D3h are rare examples of 2-aminoisobutyric acid-based 3d-4f clusters. The successful theoretical modeling of 5 yielded that the Gd-Gd exchange is of order 0.2 K, whereas the Gd-Cu exchange is an order of magnitude larger. Magnetization data collected for complex 5 yield a magnetic entropy change (−ΔSm) of 19.6 J kg−1 K−1 at 3 K and 7 T, which may be attributed to the weak magnetic interactions between the component metal ions.
The design and synthesis of a phenoxazine-based metal-organic tetrahedron (Zn4L4) as biomimetic lectin for selectively recognition of glucosamine (GlcN) was reported. Different from the free phenoxazine-based ligand (L), Zn4L4 displayed the highest fluorescent intensity enhancement efficiency toward GlcN over other related natural mono- and disaccharides. Fluorescence titration demonstrated a 1:1 stoichiometric host-guest complex was formed with an association constant about 4.03×104 L/mol. 1H NMR spectroscopic studies confirmed this selectivity resulted from the multiple hydrogen bonding interactions formed between GlcN and Zn4L4. The present results suggested that rational arrangement of recognition sites in the confined space of metal-organic cage is crucial for the selectivity toward target guests.
As a new type of two-dimensional material, MXene's unique layered structure, outstanding electrical conductivity, low density, tunable surface chemistry, and solution processability make it receive extensive attention in various fields, especially for the lightweight shielding materials since the report on electromagnetic interference (EMI) shielding of 2D Ti3C2Tx in 2016. In this review, the progress on the MXenes material including their synthetic strategies, properties and EMI application is highlighted. First, the recent advance on the different synthesis methods and properties of MXene is summarized. According to their intrinsic characteristics, the application of MXene in EMI fields is then discussed. Finally, the challenges and perspective on the future development of MXene in low-cost preparation and practical application are proposed.
The effect of cucurbit[7]uril (CB[7]) on fluorescence properties and biocompatibility of the bis-viologen biphenyl molecule (BPV22+) was investigated by using 1H NMR spectroscopy, fluorescence emission titration, and in vitro cytotoxicity experiments. CB[7] can be combined with BPV22+ in a stoichiometric ratio of 1:1 and 2:1. After the formation of host-guest complex, the fluorescence emission intensity of BPV22+ increased significantly, and the emission spectrum blue shifted. Meanwhile, the host-guest complexes showed better biocompatibility than BPV22+ in cell cytotoxicity studies. Results of this paper lay a foundation for the development of host-guest type of fluorescent probes, biological imaging and so forth.
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