Latest ArticlesImitating the signal transduction and transmembrane transport controlled by biological channels in the cell membrane, artificial nanochannels with a similar capability of sensing and transport are constructed as bionic nanochannels. To accomplish selective sensing and transport of biological analyte (as "guest"), the bionic nanochannels are modified with the artificial receptor (as "host"). Based on selective recognition between host and guest, bionic nanochannels translate the stimulus of the guest to electrochemical signal as sensors, and further regulate the transmission of guest as transporters. However, throughout all kinds of guests, the selective sensing and transport of ions and chiral molecules is a challenging problem. And throughout all hosts of ions and chiral molecules, the macrocyclic hosts with multisite of recognition show better selectivity, such as crown ethers, cyclodextrins, calixarenes, and pillararenes. In this article, we highlight recent advances in the macrocyclic host-based nanochannels for the selective sensing and transport of ionic and chiral guests, summarize the similarities and differences of different kinds of macrocyclic host-based nanochannels, and expect the research direction and application prospect.
Flexible Na-ion storage cathodes are still very few due to the challenge in achieving both reliable mechanical flexibility and excellent electrochemical performances. Herein, a new type of flexible Na3(VOPO4)2F cathode with nanocubes tightly assembled on carbon cloth is fabricated by a facile solvothermal method for the first time. The cathode is able to exhibit superior rate capability and stable cycling performance up to 1000 cycles, due to the surface-assembling of crystalline nanocubes on carbon fibers. In addition, it shows good mechanical flexibility, nearly no capacity decay is observed after continuous bending of 500 times. With this novel cathode and a directly-grown Na2Ti2O5 anode, a fully binder-free Na-ion battery is assembled. It can deliver a high working voltage and increased gravimetric energy/power densities (maximum values: 220.2 Wh/kg; 5674.7 W/kg), and can power a LED indicator at bending angles from 0° to 180°.
Acid-controlled, chemodivergent and redox-neutral annulations for the synthesis of isocoumarins and isoquinolinones have been realized via Rh(III)-catalyzed C—H activation. Diazo compounds act as a carbene precursor, and coupling occurs in one-pot process, where adipic acid and trimethylacetic acid promote chemodivergent cyclizations.
The design of pore structure is the key factor for the performance of porous carbon spheres. In this work, novel micron-sized colloidal crystal microspheres consisting of fibrous silica (F-SiO2) nanoparticles are firstly prepared by water-evaporation-induced self-assembly of F-SiO2 nanoparticles in the droplets of an inverse emulsion system to be used as sacrificial templates. Acrylonitrile (AN) was infiltrated in the voids of the F-SiO2 colloidal crystal microspheres, and in-situ induced by 60Co γ-ray to polymerize into polyacrylonitrile (PAN). After the PAN-infiltrated F-SiO2 colloidal crystal microspheres were carbonized and etched with HF solution, novel micron-sized inverse-opal N-doped carbon (IO-NC) microspheres consisting of hollow carbon nanoparticles with a hierarchical macro/meso-porous inner surface were obtained. The IO-NC microspheres have a specific surface area as high as 266.4 m2/g and a molar ratio of C/N of 5. They have a good dispersibility in water, and show a high adsorption capacity towards rhodamine B (RhB) up to 137.28 mg/(g microsphere). This work offers a way to obtain novel micron-sized hierarchical macro/meso-porous N-doped carbon microspheres, which opens a new idea to prepare high-performance hierarchical porous carbon materials.
Amorphous silicon (a-Si) is one of the most promising anode-materials for the lithium-ion battery owing to its large capacity and superior fracture resistance. However, a-Si is usually fabricated with the sophisticated chemical vapor deposition or pulse laser deposition in a limited scale. In this work, we have successfully prepared a-Si spheres (~200 nm) by reducing the TiO2-coated silica spheres with Al powders in the molten salts at 300 ℃. The coated TiO2 layer acts as a protective layer for structural maintenance during the reduction and a precursor for doping. The doped Ti element may suppress the crystal growth of Si to facilitate the formation of a-Si. The observation with in-situ transmission electron microscopy (TEM) further reveals that lithiation kinetics of the synthesized a-Si is controlled by the interfacial reaction. The Li+ diffusivity in a-Si determined from the observation is in the order of 10−14 cm2/s. The anode of a-Si spheres together with crystalline Si nanoparticles exhibits excellent electrochemical performance, delivering a reversible capacity of 1604 mAh/g at 4 A/g and a capacity retention of 78.3% after 500 cycles. The low temperature reduction process reported in this study provides a low-cost method to fabricate a-Si nanostructures as high-capacity durable anode materials
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.
Monodispersed palladium phosphide (Pd3P) (5.2 ±0.5 nm) was firstly applied to photocatalytic Suzuki coupling reaction under visible light irradiation with CdS nanoflake as a photosensitizer. This heterogeneous system exhibited high yields to corresponding products and excellent stability in alcohol solvent at room temperature.
Multiple hydrogen bonds containing nucleophilic phosphines derived from dipeptide dual-reagents catalyzed asymmetric Michael addition reactions between indene esters and activated olefins in high yields and good to excellent enantioselectivities under mild reaction conditions. The success of current highly selective reactions should provide inspiration for expansion to other reactions and would open up new paradigms for the synthesis of indanone derivatives bearing chiral quaternary carbon centers.
An unprecedented chiral secondary amine-catalyzed [3 + 3] annulation of isatin N,N'-cyclic azomethine imines with α,β-unsaturated aldehydes was developed. This strategy allowed the construction of structurally novel spiro N-heterocyclic oxindole derivatives in good yields (up to 91%) and good to excellent enantioselectivities (up to >99% ee), albeit with modest diastereoselectivities (up to 3.1:1 dr).
Circulating tumor DNA (ctDNA) refers to a class of acellular nucleic acids carrying genetic features of primary tumor, which can be regarded as a promising noninvasive biomarker for cancer diagnosis. The development of ctDNA assay is an important component of liquid biopsy. In this study, we have fabricated a novel electrochemical strategy for ultrasensitive detection of ctDNA combining the merits of strand displacement amplification and DNA nanostructures. Stable DNA triangular prism is firstly self-assembled and modified on the electrode surface. After target initiated strand displacement polymerization reaction, the generated DNA product helps the formation of three-way junction nanostructure on triangular prism, which localizes electrochemical species. By carefully investigating the electrochemical responses, the limit of detection (LOD) for ctDNA assay as low as 48 amol/L is achieved. This proposed electrochemical biosensor shows great potential for clinical applications.
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