Latest ArticlesFunctional materials with multiple properties are urgent to be explored to reach high requirements for applications nowadays. In this work, a new multifunctional one-dimensional (1D) chain compound [N(C3H7)4][Cu(ohpma)]·H2O 1 (ohpma = deprotonated N-(2-hydoxyphenyl)oxamic acid) exhibiting both 1D antiferromagnetic and nonlinear optical properties, which are both originated from the same polar [Cu(C8H4NO4)] magnetic units, has been successfully synthesized by evaporation at room temperature. Bis-polydentate nature of the (ohpma)3− ligand with constrained tridentate and bidentate coordination sites conducts Cu2+ ions coordinating in different geometries and forms 1D chains along the c axis, which are further separated by the [N(C3H7)4]+ cations. And the 1D magnetic chains further exhibit noncentrosymmetric polar arrangement. Nonlinear optical study shows polar compound 1 exhibits a discernible second-harmonic generation (SHG) efficiency and the calculation of the partial density of states indicates that the SHG efficiency of 1 is mainly originated from the polar [Cu(C8H4NO4)] magnetic units. Moreover, magnetic susceptibility shows a broad maximum around 70 K with strong intrachain interaction of J/kB = −113.0 K but no long-range order is observed down to 2 K, suggesting that 1 shows a good 1D magnetism. Both good 1D magnetism and SHG activity suggest that 1 could be as a potential multifunctional material, particularly.
Membrane permeability and intracellular diffusion of fluorescent probes determine staining selectivity of intracellular substructures. However, the relationship between the molecular structure of fluorescent probes and their membrane permeability and intracellular distribution is poorly understood. In this paper, we reported a series of 1,8-naphthalimide dyes and carried out cell imaging experiments, and found that the presence of amino hydrogen in these dyes played a crucial role in their cell membrane permeability and intracellular distribution. The secondary amino group containing compounds 1–4 show excellent membrane permeability and strong fluorescence in living cells. While the tertiary amine containing dyes 5 and 6 can hardly permeate the cell membrane though they show extremely similar structure with compounds 2–4. Compound 1 can selectively image lipid droplets by selecting the wavelength of excitation light. With the specificity for lysosomes, 2 and 4 have been used in long-term time-lapses imaging of lysosomal dynamics and tracking the process of lysosome–lysosome interaction, fusion and movement. The effect of hydrogen-containing amino substituent on the cell membrane permeability of fluorescent molecules is promising for the development of better biocompatible probes.
Targeting delivery of tumor-associated carbohydrate antigen (TACA)-based vaccine to antigen-presenting cells (APCs) mediated by endogenous antibodies can improve the immunogenicity of TACA. However, an essential requirement of this approach is to generate high titers of endogenous antibodies in vivo through pre-immunization, which complicates the immunization procedure and may cause side effects. Herein, we report a new generation of APC-targeting TACA-based supramolecular complex vaccine, assembled by sialyl Thomsen-nouveau-bovine serum albumin-adamantine (sTn-BSA-Ada) and heptavalent rhamnose (Rha)-modified β-cyclodextrin (β-CD) via host–guest interaction. The complex vaccine retained anti-Rha antibodies recruiting capability and facilitated the APCs uptake of the vaccine via the interaction of the Fc-domain with the Fc receptors on APCs. We demonstrate that direct immunization of complex vaccine elicited anti-Rha and anti-sTn specific immune response synchronously, generating a novel self-enhancement effect that can improve the antigen delivery to APCs in high efficacy. The structure–activity relationship (SAR) study proved that complex vaccine 4 with polyethylene glycol 6 (PEG6) linker in host molecule provoked a robust and specific sTn immune response comparable to the pre-immunization approach. The antisera induced by complex vaccine, either through direct immunization or pre-immunization, exhibited equal potency of cytotoxicity against the sTn expression cancer cells. This study provides a general platform for TACA-based vaccines with self-enhancement effects without the need for pre-immunization.
Passive daytime radiative cooling (PDRC) technology is emerging as one of the most promising solutions to the global problem of spacing cooling, but its practical application is limited due to reduced cooling effectiveness caused by daily wear and tear, as well as dirt contamination. To tackle this problem, we report a novel strategy by introducing a renewable armor structure for prolonging the anti-fouling and cooling effectiveness properties of the PDRC coatings. The armor structure is designed by decorating fluorinated hollow glass microspheres (HGM) inside rigid resin composite matrices. The HGM serve triple purposes, including providing isolated cavities for enhanced solar reflectance, reinforcing the matrices to form robust armored structures, and increasing thermal emittance. When the coatings are worn, the HGM on the surface expose their concave cavities with numerous hydrophobic fragments, generating a highly rough surface that guarantee the superhydrophobic function. The coatings show a high sunlight reflectance (0.93) and thermal emittance (0.94) in the long-wave infrared window, leading to a cooling of 5 ℃ below ambient temperature under high solar flux (~900 W/m2). When anti-fouling functions are reduced, they can be regenerated more than 100 cycles without compromising the PDRC function by simple wearing treatment. Furthermore, these coatings can be easily prepared using a one-pot spray method with low-cost materials, exhibit strong adhesion to a variety of substrates, and demonstrate exceptional environmental stability. Therefore, we anticipate their immediate application opportunities for spacing cooling.
Herein, a site-selective paired electrochemical C–H oxidation of functionalized alkyl arenes promoted by nickel catalyst is disclosed. A Ni(Ⅱ)-dioxygen species formed in situ efficiently enable the oxidation process under mild conditions with a broad substrate scope with excellent functional group compatibilities, such as free carboxylic acid, aldehyde, halogen (including aryl iodide), amide and amino acid. The use of the nickel catalyst in combination with water provides a safe, green and economical method for oxidation of a range of molecules varying in complexity and drug derivatives, demonstrating its potential application in organic synthesis and the pharmaceutical industry. Reaction outcomes and mechanistic studies revealed the key role of the in situ Ni(Ⅱ)-dioxygen species for the subsequent oxidation of C(sp3)–H bonds, and short-lived reactive intermediates (aryl radical cation) was rapidly captured by the combination of a bipolar ultramicroelectrode (BUME) with nano-electrospray ionization mass spectrometry.
In order to solve the contradiction between the rapidly growing energy demand and the excessive exploitation of fossil fuels, it is urgent to research and develops more environmentally friendly and efficient energy storage technologies. Therefore, the development of high-performance cathode materials to enhance the energy density of SIB is currently one of the most important topics of scientific research. Advanced high-voltage and low-cost cathode material for SIBs, a composite of carbon-coated Na4MnCr(PO4)3 (NASICON-type), polyvinylpyrrolidone (PVP), and modified carbon nanotubes (CNTs) is prepared by sol-gel and freeze-drying method. Due to the high conductivity of CNTs, the conductivity of the composite is significantly improved, and its initial capacity is increased to 114 mAh/g at 0.5 C and 96 mAh/g at 5 C (Mn2+/Mn4+ conversion for voltage windows 1.4-4.3 V). Moreover, the multi-electrons transfer of Cr3+/Cr4+ and Mn2+/Mn4+ can provide a high capacity of 165 mAh/g at 0.1 C and 102 mAh/g at 5 C in the high voltage window of 1.4-4.6 V. Furthermore, PVP can effectively inhibit the Jahn-Teller effect caused by Mn ion, making the composite have more excellent high-rate performance and stability. In addition, GITT, EIS and CV curves were drawn to better reveal the excellent kinetic properties of Na4MnCr(PO4)3@C@PVP@CNT cathode, and the mechanism of its performance improvement is deeply studied and discussed. Accordingly, the co-doping of CNTs and PVP is a simple way to high conductivity and fast charging of cathode materials for SIBs.
Photodynamic therapy (PDT) is an effective treatment method for tumors. But the specifically accumulated of photosensitizer was very difficult in the tumor site, which greatly limited the efficacy of PDT. Here, mitochondria-targeted Janus mesoporous nanoplatform (JPMO-Pt-CTPP-ZnPc) for PDT was prepared, the nanoplatform has uniform size (275 nm) and good dispersion and biocompatibility. The confocal laser scanning microscopy (CLSM) revealed the signal of ZnPc of JPMO-Pt-CTPP-ZnPc were higher than JPMO-Pt-ZnPc in tumor cells, and flow cytometry results showed the cell uptake efficiency of JPMO-Pt-CTPP-ZnPc was 2.5-fold higher than that of JPMO-Pt-ZnPc. This revealed the modification of CTPP significantly improves the targeting ability of the nanoplatform. In vitro anti-tumor experiment showed the JPMO-Pt-CTPP-ZnPc significantly inhibited the growth of tumor cells upon the irradiation of low-power laser, and the survival rate of cells incubated with 60 µg/mL JPMO-Pt-CTPP-ZnPc was only 3%. Simultaneously, compared with JPMO-Pt-ZnPc (not modified with mitochondria targeting molecules CTPP), the PDT efficacy of JPMO-Pt-CTPP-ZnPc was significantly better, as it has targeted mitochondria in cells.
Although it has been developed for many years, nucleic acid aptamer screening technology still fails to be widely used, a considerable part of it is due to the variability of tumor cell morphology, which leads to the use of immortalized cell lines in the laboratory to screen nucleic acid aptamers for recognition ability of tumor cells in the diseased body. To address this, primary cells that can be stably passaged were isolated and extracted from spontaneous tumors of genetically engineered pancreatic ductal adenocarcinoma model mice in this study. Next, an automated screening instrument for nucleic acid aptamers developed autonomously by our group was used to perform efficient aptamer screening using a limited number of cells, and the obtained nucleic acid aptamers were affinity verified at the cellular level. Finally, to answer the question of the cell growth environment difference on the recognition ability of nucleic acid aptamers, we verified its targeting ability to tumors in vivo on a nude mice xenograft tumor model, and further used a common antitumor drug doxorubicin combined with nucleic acid aptamers to verify the drug loading ability of this aptamer combined with the targeting therapeutic ability.
The design and development of energy storage device with high energy/power density has become a research hotspot. Zinc-ion hybrid capacitors (ZHCs) are considered as one of the most promising candidates. However, the application of ZHCs is hindered by their low energy density at high power density due to the unsatisfactory cathode material. In this study, a novel 3D phosphorus-doped carbon nanotube/reduced graphene oxide (P-CNT/rGO) aerogel cathode is synthesized through a synergistic modification strategy of CNT insertion and P doping modification combined with 3D porous design. The as-obtained P-CNT/rGO aerogel cathode manifests significantly increased surface aera, expanded interlayer spacing, and enhanced pseudocapacitance behavior, thus leading to significantly enhanced specific capacitance and superb ions transport performance. The as-assembled ZHC based on P-CNT/rGO cathode delivers a superior energy density of 42.2 Wh/kg at an extreme-high power density of 80 kW/kg and excellent cycle life. In-depth kinetic analyses are undertaken to prove the enhanced pseudocapacitance behavior and exceptional power output capability of ZHCs. Furthermore, the reaction mechanism of physical and chemical adsorption/desorption of electrolyte ions on the P-CNT/rGO cathode is revealed by systematic ex-situ characterizations. This work can provide a valuable reference for developing advanced graphene-based cathode for high energy/power density ZHCs.
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