Latest ArticlesThe sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have always restricted the development of lithium oxygen batteries (LOBs). Herein, hollow carbon spheres loaded with Pd/Pd4S heterostructure (Pd/Pd4S@HCS) were successfully prepared via the in-situ deposition to improve the electrocatalytic activities for both ORR and OER in LOBs. With the well-dispersed Pd/Pd4S nanoparticles, the hierarchical composite with large specific surface area offers favorable transport channels for ions, electron and oxygen. Especially, the Pd/Pd4S nanoparticles could exhibit excellent electrochemical performance for ORR and OER due to their intrinsic catalytic property and interfacial effect from the heterostructure. Therefore, the LOBs with Pd/Pd4S@HCS as cathode catalyst show improved specific capacities, good rate ability and stable cycling performance.
Amino group protective strategy has consequently emerged in multistep organic synthesis. Easy and selective deprotection procedures are crucial to facilitate the chemical transformation. Recently, Zhang's group from Henan Normal University collaborating with Chen's group of Nankai University developed a novel strategy for the regiospecific cleavage of inert aryl C—N bonds in N-aryl amides by hypervalent iodine(V) reagents. These procedures allow removal of sort of aryl groups under mild conditions to give primary amides in high efficiency. It bestows these aryl groups with the characteristics of amino protecting groups that might be the supplement of amino protecting group chemistry.
Physical adsorption is a common method to solve the contamination of methylene blue in dyeing wastewater. As a kind of adsorption material, cellulose aerogels with high porosity and surface areas have great potential application in methylene blue removal. However, the week hydrogen bonding between cellulose nanofibers making the cellulose aerogels with the poor mechanical properties and can be easily destroyed during adsorption. Hence, the preparation of cellulose aerogels with high mechanical strength is still a great challenge. Here, we report a robust super-assembly strategy to fabricate cellulose aerogels by combining cellulose nanofibers with PVA and M-K10. The resulting cellulose aerogels not only has a robust chemically cross-linked network, but also has strong H-bonds, which greatly enhance the mechanical properties. The resulting cellulose aerogels possess a low density of 19.32 mg/cm3. Furthermore, the cellulose aerogel shows 93% shape recovery under 60% strain (9.5 kPa under 60% strain) after 100 cycles, showing excellent mechanical property. The adsorption capacity of cellulose aerogel to methylene blue solution of 20 mg/L is 2.28 mg/g and the adsorption kinetics and adsorption isotherms have also been studied. Pseudo-second-order kinetic model and Freundlich isotherm model are more acceptable for indicating the adsorption process of methylene blue on the cellulose aerogel. Thus, this compressible and durable cellulose aerogel is a very prospective material for dyeing wastewater cleanup.
It is well known that zero-valent iron (ZVI) could catalyze the oxidation of various oxidants to realize the rapid oxidation removal of pollutants. However, in this study, we found that the addition of different oxidants could regulate the redox function of ZVI system. In three different co-treatment systems, the effects of different oxidizers (peroxymonosulfate (PMS), persulfate (PDS), hydrogen peroxide (H2O2)) dosages on the ratios of oxidative degradation rate and reductive degradation rate of p-nitrophenol (PNP) were studied. The effect of the H+ released from oxidizers and the generated reactive oxygen species (ROS) in ZVI/PMS, ZVI/PDS, ZVI/H2O2 systems were detailed discussed. Especially, the contribution of generated ROS for reductive degradation of PNP was quantified in the ZVI/H2O2 system. Based on the results of TOC removal, UV–vis absorption spectra, and intermediates concentration curves, it was found that the degradation of PNP changed from reduction to oxidation with the increase of oxidant proportion. When the molar ratio of ZVI to oxidizer equal to 100, PNP was mainly degraded by reduction accompanied by slight oxidation. Combined with the results of SEM-EDS and XPS, it was confirmed that the enhanced degradation of PNP under the addition of oxidant was mainly related to the generated ROS, the additional H+, and the corrosion products of ZVI.
Amphichoterpenoids A–C (1–3), unprecedented picoline-derived meroterpenoids possessing a pyrano[3, 2-c]pyridinyl-γ-pyranone scaffold, were characterized from the ascidian-derived fungus Amphichorda felina SYSU-MS7908. Their structures were elucidated by spectroscopic methods, X-ray diffraction and electronic circular dichroism (ECD) calculations. A plausible biosynthetic pathway was proposed. The isolated compounds displayed moderate inhibitory activity against acetylcholinesterase with 50% inhibiting concentration (IC50) values of 18.8–53.2 μmol/L.
The electrocatalysis of nitrate reduction reaction (NRR) has been considered to be a promising nitrate removal technology. Developing a highly effective iron-based electrocatalyst is an essential challenge for NRR. Herein, boron-iron nanochains (B-Fe NCs) as efficient NRR catalysts were prepared via a facile low-cost and scalable method. The Fe/B ratio of the B-Fe NCs-x can be elaborately adjusted to optimize the NRR catalytic performance. Due to the electron transfer from boron to metal, the metal-metal bonds are weakened and the electron density near the metal atom centers are rearranged, which are favor of the conversion from NO3- into N2. Moreover, the well-crosslinked chain-like architectures benefit the mass/electron transport to boost the exposure of abundant catalytic active sites. Laboratory experiments demonstrated that the optimized B-Fe NCs catalyst exhibits superior intrinsic electrocatalytic NRR activity of high nitrate conversion (~80%), ultrahigh nitrogen selectivity (~99%) and excellent long-term reactivity in the mixed electrolyte system (0.02 mol/L NaCl and 0.02 mol/L Na2SO4 mixed electrolyte), and the electrocatalytic activity of the material shows poor performance at low chloride ion concentration (Nitrate conversion of ~61% and nitrogen selectivity of ~57% in 0.005 mol/L NaCl and 0.035 mol/L Na2SO4 mixed electrolyte). This study provides a broad application prospect for further exploring the high-efficiency and low-cost iron-based functional nanostructures for electrocatalytic nitrate reduction.
The remarkable development of nanotechnology and nanoscience has greatly promoted the vigorous development of the field of nanomaterials. This study explores a porous cuboid Ni/NiO composite nanomaterial obtained by calcining NiC2O4·2H2O under a N2 environment. The composite affords direct electrochemical activity and good electrocatalytic properties. Compared to uncalcined precursor, the porous Ni/NiO obtained after calcination exhibited higher catalytic activity for glucose oxidation with higher sensitivity. Moreover, because of its regular cube structure the as-synthesized Ni/NiO exhibited improved electrochemical stability. Such porous Ni/NiO nanocubes represent promising glucose catalyst with high sensitivity and selectivity, improved stability and fast amperometric response.
A nitro group is a common fluorescence quencher, but its quenching efficiency can be easily affected by the surrounding environment. To date, there has been no systematic study on the effects of electron-withdrawing groups on the quenching efficiency of nitro groups. Herein, by virtue of experimental validation and theoretical calculations, we found that strong electron-withdrawing groups, such as pyridinium and dicyanovinyl groups, are detrimental to the quenching effect of nitro groups. Decreasing the electron-withdrawing ability could restore the nitro group's quenching effect.
An enzyme-responsive polysaccharide supramolecular targeted nanoassembly was successfully constructed by the host-guest complexation of positively charged mono-(6-(tetraethylenepentamine)-6-deoxy)-β-cyclodextrin (TEPA-CD) with adamantane-grafted hyaluronic acid (HA-ADA). Possessing a series of positively charged polyamine chains, the obtained polysaccharide nanoassembly could serve as a biocompatible plasmid DNA (pDNA) container. More interestingly, the pDNA could be released from the nanoassembly through the enzymatic degradation of HA skeleton, which realized the controlled pDNA binding and release. Besides, the polysaccharide nanoassembly exhibited lower cytotoxicity than the commercial transfection reagents 25kDa bPEI (PEI25k), accompanied by similar gene delivery effect. We believe that this work might present a convenient method for targeted, controlled gene delivery.
Green and recyclable solid acid catalysts are in urgent demand as a substitute for conventional liquid mineral acids. In this work, a series of novel sulfonic acid-functionalized core-shell Fe3O4@carbon microspheres (Fe3O4@C-SO3H) have been designed and synthesized as an efficient and recyclable heterogeneous acid catalyst. For the synthesis, core-shell Fe3O4@RF (resorcinol-formaldehyde) microspheres with tunable shell thickness were achieved by interfacial polymerization on magnetic Fe3O4 microspheres. After high-temperature carbonization, the microspheres were eventually treated by surface sulfonation, resulting in Fe3O4@C-x-SO3H (x stands for carbonization temperature) microspheres with abundant surface SO3H groups. The obtained microspheres possess uniform core-shell structure, partially-graphitized carbon skeletons, superparamagnetic property, high magnetization saturation value of 10.6 emu/g, and rich SO3H groups. The surface acid amounts can be adjusted in the range of 0.59–1.04 mmol/g via sulfonation treatment of carbon shells with different graphitization degrees. The magnetic Fe3O4@C-x-SO3H microspheres were utilized as a solid acid catalyst for the acetalization reaction between benzaldehyde and ethylene glycol, demonstrating high selectivity (97%) to benzaldehyde ethylene glycol acetal. More importantly, by applying an external magnetic field, the catalysts can be easily separated from the heterogeneous reaction solutions, which later show well preserved catalytic activity even after 9 cycles, revealing good recyclability and high stability.
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