溶剂比对Mn-ZnO复合纳米线形貌及吸附脱硫研究

采用水热法合成了Mn-ZnO复合纳米线,通过改变溶剂比来考察其对Mn-ZnO形貌的影响,并用等体积浸渍法负载金属Ni,制备反应吸附脱硫剂,以正庚烷/噻吩为模拟油并在固定床反应器装置上评价反应吸附脱硫性能.通过XRD、BET、SEM等方法对该催化剂进行表征;研究表明:溶剂比不同可导致Mn-ZnO复合物形貌的不同,从而影响脱硫性能.以乙醇溶液为溶剂制备的脱硫催化剂脱硫率可达99;左右,并且具有良好的稳定性.     

Effect of the topology on the antibacterial activity of cationic polythioether synthesized by all-click chemistry

Cationic compounds often serve as antibacterial materials for a wide range of applications. However, the relationship of topology−antibacterial activity has been rarely revealed. Herein, three cationic polythioethers (CPTEs) with hyperbranched topologies are well designed and facilely synthesized via an all-click chemistry strategy (including thiol-ene and epoxy-amine additions). These as-prepared CPTEs were found to exhibited outstanding antibacterial activity against Escherichia coli and Staphylococcus aureus with minimum inhibitory concentrations against E. coli of 7.3, 14.6, and 14.6 μg ml⁻¹, and against S. aureus of 14.6, 29.2, and 29.2 μg ml⁻¹, respectively. The antibacterial activity is coincident with their degree of branching (DB, their DB values of 0.81, 0.48, and 0.27), which is mainly attributed to the inherent three-dimensional structure. The present strategy reveals the relationship of polymer topology and antibacterial activity, providing a novel possibility for designing and/or synthesis of high-efficiency antibacterial agents.     

Sulfonated poly(ether ether ketone) composite membranes based on amino-modified halloysite nanotubes that effectively immobilize phosphotungstic acid

In this work, we prepared amino-modified halloysite nanotubes (PEI-DHNTs) via the co-deposition of self-polymerized dopamine and polyethylenimine (PEI) on the surface of nanotubes, which was confirmed by X-ray photoelectron spectroscopy (XPS) and Thermogravimetric analysis (TGA). A series of composite proton exchange membranes (PEMs) were prepared by incorporating PEI-DHNTs and phosphotungstic acid (HPW) into sulfonated poly(ether ether ketone) (SPEEK). It was found that both PEI-DHNTs and HPW were well dispersed in the polymer matrix, exhibiting excellent filler-matrix compatibility. The composite membranes demonstrated enhanced proton conductivity, reaching as high as 0.078 S cm⁻¹ with 33.3 wt.% HPW loading, which was ~90% higher than that of SPEEK control membrane. Such improvement was mainly attributed to the strong acid–base pairs formed by PEI-DHNT with both SPEEK and HPW, which shortened proton hopping distance and created more continuous proton conduction pathways. Furthermore, the membrane conductivity remained almost constant after 1 year's immersion in liquid water, indicating the successful immobilization of HPW in the composite membranes.     

Interfacial Engineering FeOOH/CoO Nanoneedle Array for Efficient Overall Water Splitting Driven by Solar Energy

Interface engineering has been applied as an effective strategy to boost the electrocatalytic performance because of the strong coupling and synergistic effects between individual components. Here, we engineered vertically aligned FeOOH/CoO nanoneedle array with a synergistic interface between FeOOH and CoO on Ni foam (NF) by a simple impregnation method. The synthesized FeOOH/CoO exhibits outstanding electrocatalytic activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in an alkaline medium. For the overall water splitting, the bifunctional FeOOH/CoO nanoneedle catalyst requires only a cell voltage of 1.58 V to achieve a current density of 10 mA cm⁻², which is much lower than that required for IrO₂//Pt/C (1.68 V). The FeOOH/CoO catalyst has been successfully applied for solar cell-driven water electrolysis, revealing its great potential for commercial hydrogen production and solar energy storage.     

Continuous Electrochemical Synthesis of Iso-Coumarin Derivatives from o-(1-Alkynyl) Benzoates under Metal- and Oxidant-Free

A non-oxidant and metal-free strategy for synthesizing iso-coumarin by using a continuous electrochemical microreactor to initiate an oxidative cyclization reaction of o-(1-alkynyl) benzoate and radicals. This efficient and clean continuous electrosynthesis method not only avoids the complicated gas protection operation and production of by-products in the batch processes, but also help to overcome the difficulty that batch metal catalysis and electrocatalysis are difficult to scale up, and has the potential for pilot-scale experiment.     

Journey from Small-Molecule Diyne Structures to 2D Graphdiyne: Synthetic Strategies

Graphdiyne (GDY) exhibits unique characteristics of a highly conjugated π system, evenly distributed nanopores, and a direct band gap. This has encouraged multidisciplinary research groups to investigate its application in energy conversion and storage, catalysts, electronic devices, sensing, and separation. Herein, the achievements of synthetic strategies for preparing small-molecule diyne structures (GDY substructure), 1D nanoribbons, and 2D GDY are presented. These studies may help future investigations into the basic structure-related properties of GDY and synthetic methodology for the future developments of GDY-related 2D carbon materials.     

Directed Gas Phase Formation of Silene (H2SiCH2)

The silene molecule (H₂SiCH₂; X¹A₁) has been synthesized under single collision conditions via the bimolecular gas phase reaction of ground state methylidyne radicals (CH) with silane (SiH₄). Exploiting crossed molecular beams experiments augmented by high-level electronic structure calculations, the elementary reaction commenced on the doublet surface through a barrierless insertion of the methylidyne radical into a silicon-hydrogen bond forming the silylmethyl (CH₂SiH₃; X²A′) complex followed by hydrogen migration to the methylsilyl radical (SiH₂CH₃; X²A′). Both silylmethyl and methylsilyl intermediates undergo unimolecular hydrogen loss to silene (H₂SiCH₂; X¹A₁). The exploration of the elementary reaction of methylidyne with silane delivers a unique view at the widely uncharted reaction dynamics and isomerization processes of the carbon–silicon system in the gas phase, which are noticeably different from those of the isovalent carbon system thus contributing to our knowledge on carbon silicon bond couplings at the molecular level.     

Supramolecular Assembly of TPE-Based Glycoclusters with Dicyanomethylene-4H-pyran (DM) Fluorescent Probes Improve Their Properties for Peroxynitrite Sensing and Cell Imaging

Two red-emitting dicyanomethylene-4H-pyran (DM) based fluorescent probes were designed and used for peroxynitrite (ONOO⁻) detection. Nevertheless, the aggregation-caused quenching effect diminished the fluorescence and restricted their further applications. To overcome this problem, tetraphenylethylene (TPE) based glycoclusters were used to self-assemble with these DM probes to obtain supramolecular water-soluble glyco-dots. This self-assembly strategy enhanced the fluorescence intensity, leading to an enhanced selectivity and activity of the resulting glyco-dot comparing to DM probes alone in PBS buffer. The glyco-dots also exhibited better results during fluorescence sensing of intracellular ONOO⁻ than the probes alone, thereby offering scope for the development of other similar supramolecular glyco-systems for chemical biological studies.     

Enzymatic Insertion of Lipids Increases Membrane Tension for Inhibiting Drug Resistant Cancer Cells

Although lipids contribute to cancer drug resistance, it is challenging to target diverse range of lipids. Here, we show enzymatically inserting exceedingly simple synthetic lipids into membranes for increasing membrane tension and selectively inhibiting drug resistant cancer cells. The lipid, formed by conjugating dodecylamine to d -phosphotyrosine, self-assembles to form micelles. Enzymatic dephosphorylation of the micelles inserts the lipids into membranes and increases membrane tension. The micelles effectively inhibit a drug resistant glioblastoma cell (T98G) or a triple-negative breast cancer cell (HCC1937), without inducing acquired drug resistance. Moreover, the enzymatic reaction of the micelles promotes the accumulation of the lipids in the membranes of subcellular organelles (e.g., endoplasmic reticulum (ER), Golgi, and mitochondria), thus activating multiple regulated cell death pathways. This work, in which for the first time membrane tension is increased to inhibit cancer cells, illustrates a new and powerful supramolecular approach for antagonizing difficult drug targets.