Synthesis and Fluorescent Performance of Fluorescein-functionalized Waterborne Polyurethane

A novel yellow fluorescent diisocyanate 3,6-di(hexamethylene urethano)spiro[xanthene-9,3′-phthalide] diisocyanate (DIX) was synthesized by the reaction of fluorescein with hexamethylene diisocyanate first. Using DIX to substitute partially isophorone diisocyanate (IPDI), a kind of yellow fluorescent waterborne polyurethane DIX-WPU was prepared by blocking the fluorophore of DIX into the polyurethane chain using IPDI, polytetramethylene ether glycol and 2,2-dimethylol propionic acid. The molecular structure of DIX and DIX-WPU was confirmed by means of Fourier transform infrared spectroscopy. The fluorophore is fixed permanently in the polyurethane chain and is difficult to migrate due to the covalent bonding with other component during the synthesis. The fluorescence intensity of DIX-WPU fluorescent dispersion was enhanced greatly comparing with that of fluorescein in a wide range of fluorophore content between 1 × 10^–7 and 1 × 10^–3 mol/L. The fluorescence of DIX-WPU dispersion is very stable not only for the long term storage but also for the fluorescence quencher. It was found that the fluorescence intensity of DIX-WPU increased with the increase of temperature.     

Porous Microstructured Surfaces with pH‐Triggered Antibacterial Properties

New antibacterial films are designed with the capability to reversibly regulate their killing and repelling functions in response to variations in environmental pH. These systems consist of porous polystyrene surfaces as the main components and a copolymer bearing pH‐sensitive thiazole and triazole groups as the minor components. These pH‐sensitive groups, located on the surfaces, can be partially protonated at acidic pH levels, increasing the positive charge density of the surfaces and their antibacterial activity. Similarly, their bacterial adhesion and killing efficiencies in response to changes in pH are evaluated by analyzing the bacterial viability of Staphylococcus aureus bacteria on the surfaces under acidic and neutral pH values. It is demonstrated that after only 1 h of incubation with the bacterial suspension in acidic conditions, the surfaces killed the bacteria, while at pH = 7.4, some of the adhered bacteria are removed. Furthermore, the surface topography exerts an important role by intensifying this response.     

硫磺素型聚乳酸/苯磺酸室温磷光体系的构建

在硫磺素上分别引入给电子基氧、 硫和甲氧基, 合成出2-[4-(苯并噻唑-2-基)苯氧基]乙-1-醇(BT-OH)、 2-{[4-(苯并噻唑-2-基)苯基]硫代}乙-1-醇(BT-SH)和2-[4-(苯并噻唑-2-基)-2-甲氧基苯氧基]乙-1-醇(BT-M-OH) 3种硫磺素衍生物. 利用硫磺素衍生物作为引发剂引发D,L-丙交酯聚合, 得到3种硫磺素型聚乳酸, 再加入苯磺酸, 构建出可在室温下产生磷光的硫磺素型聚乳酸/苯磺酸体系, 实现了从荧光到磷光的可调分子发射, 其中磷光寿命最长达108.19 ms. 研究发现, 引入苯磺酸会使硫磺素型聚乳酸产生分子内电荷转移态, 质子化效应导致绿色和橘色的磷光发射.     

Polymer Nanodiscs and Their Bioanalytical Potential

Membrane proteins (MPs) play a pivotal role in cellular function and are therefore predominant pharmaceutical targets. Although detailed understanding of MP structure and mechanistic activity is invaluable for rational drug design, challenges are associated with the purification and study of MPs. This review delves into the historical developments that became the prelude to currently available membrane mimetic technologies before shining a spotlight on polymer nanodiscs. These are soluble nanosized particles capable of encompassing MPs embedded in a phospholipid ring. The expanding range of reported amphipathic polymer nanodisc materials is presented and discussed in terms of their tolerance to different solution conditions and their nanodisc properties. Finally, the analytical scope of polymer nanodiscs is considered in both the demonstration of basic nanodisc parameters as well as in the elucidation of structures, lipid–protein interactions, and the functional mechanisms of reconstituted membrane proteins. The final emphasis is given to the unique benefits and applications demonstrated for native nanodiscs accessed through a detergent free process.     

Advanced porous organic materials for sample preparation in pharmaceutical analysis

The development of novel sample preparation media plays a crucial role in pharmaceutical analysis. To facilitate the extraction and enrichment of pharmaceutical molecules in complex samples, various functionalized materials have been developed and prepared as adsorbents. Recently, some functionalized porous organic materials have become adsorbents for pharmaceutical analysis due to their unique properties of adsorption and recognition. These advanced porous organic materials, combined with consequent analytical techniques, have been successfully used for pharmaceutical analysis in complex samples such as environmental and biological samples. This review encapsulates the progress of advanced porous materials for pharmaceutical analysis including pesticides, antibiotics, chiral drugs, and other compounds in the past decade. In addition, we also address the limitations and future trends of these porous organic materials in pharmaceutical analysis.     

Alkylation of cycloalkano[B]indoles via indolylmagnesium salts: Synthesis of 3h-indoles and oxidative rearrangement to spiro[cycloalkane-1,2′-indolin]-3′-ones

Alkylation of cycloalkano[b]indolylmagnesium iodide with alkyl halides has been analyzed to prepare cycloalkano-3H-indoles, methyl and N,N-dimethylpropyl derivatives. Spiro[cycloalkane-1,2′-indolin-3′-one] derivatives appear as secondary products in this reaction. Selectivity and optimization of the reaction has been determined and a mechanism for the formation of the spiro derivative is proposed.     

Electrocatalytic Urea Synthesis with 63.5 % Faradaic Efficiency and 100 % N-Selectivity via One-step C−N coupling

Electrocatalytic urea synthesis via coupling N₂ and CO₂ provides an effective route to mitigate energy crisis and close carbon footprint. However, the difficulty on breaking N≡N is the main reason that caused low efficiencies for both electrocatalytic NH₃ and urea synthesis, which is the bottleneck restricting their industrial applications. Herein, a new mechanism to overcome the inert of the nitrogen molecule was proposed by elongating N≡N instead of breaking N≡N to realize one-step C−N coupling in the process for urea production. We constructed a Zn−Mn diatomic catalyst with axial chloride coordination, Zn−Mn sites display high tolerance to CO poisoning and the Faradaic efficiency can even be increased to 63.5 %, which is the highest value that has ever been reported. More importantly, negligible N≡N bond breakage effectively avoids the generation of ammonia as intermediates, therefore, the N-selectivity in the co-electrocatalytic system reaches100 % for urea synthesis. The previous cognition that electrocatalysts for urea synthesis must possess ammonia synthesis activity has been broken. Isotope-labelled measurements and Operando synchrotron-radiation Fourier transform infrared spectroscopy validate that activation of N−N triple bond and nitrogen fixation activity arise from the one-step C−N coupling process of CO species with adsorbed N₂ molecules.     

超高温(200-250 ℃)聚合物电解质膜燃料电池的机遇与挑战

低温质子交换膜燃料电池的商业化受到高纯度氢气制取、储存、运输及加注的制约。将燃料电池工作温度提高到200-250 ℃可显著提高电极动力学,提高对一氧化碳等杂质气体的耐受性,降低氢气制取成本,简化水和热管理,为燃料电池提供更多燃料选择,使得高温质子交换膜燃料电池有望实现原位甲醇重整制氢系统与燃料电池系统的无温差耦合,同时较高的运行温度为直接甲醇燃料电池和非贵金属催化剂替代铂基催化剂提供了有利条件。但超高温（200-250 ℃）聚合物电解质膜燃料电池的发展依然面临着艰巨的挑战,为促进超高温聚合物电解质膜燃料电池的发展,本文将系统总结近年的相关进展,探讨超高温聚合物电解质膜燃料电池面临的机遇与挑战。