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.
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.
The preparation of medium-sized benzo[b]azocines has always been challenging because of inherently unfavorable enthalpy and entropy factors. This report presents a novel approach for accessing 8-membered seleno-benzo[b]azocines via electrochemically-driven seleno-cyclization. This method enables room-temperature preparation of various structurally diverse medium-sized seleno-benzo[b]azocines. The facile deselenation of the seleno-cyclization products to generate functionalized dienes is an additional benefit of this indispensable reaction. Mechanistic insights are presented based on radical inhibition experiments and cyclic voltammetry measurements, which elucidate the radical pathway. Finally, density functional theory calculations further rationalize the rate-determining step and the unique chemoselectivity observed in this transformation.
Saccharide sensing is a very meaningful research topic as saccharides are involved in many biological activities. However, it is challenging to design molecular sensors for saccharides because this family of compounds is hydromimetic in aqueous solutions and shares a similar chemical structure. In this review, research progress in the development of porphyrin-based saccharide sensors is described with representative examples. We focus on using porphyrin as the signal reporter because porphyrins exhibit unique advantages in high chemical stability, long emission wavelength, and multiple structural modification strategies. Reported literature results have been classified into mainly two sections according to the general working principles of the porphyrin sensor molecules. In the first section, recognition unit, design strategy and sensing performance of traditional porphyrin-based selective saccharide sensors are discussed. While in the second section, development of porphyrin-based sensor arrays for pattern recognition of saccharides has been summarized. Looking through the design strategy and sensing performance of reported achievements, it is reasonable to anticipate a bright future for designing practical porphyrin-based saccharide sensors.
Nitrate (NO3−) electroreduction reaction (NO3−RR) provides an attractive and sustainable route for NO3− pollution mitigation or energy-saved ammonia (NH3) synthesis. In this work, high-quality B and Fe co-doped Co2P hollow nanocubes (B/Fe-Co2P HNCs) are successfully synthesized though simultaneous boronation-phosphorization treatment, which reveal outstanding selectivity, activity, stability for the NO3− to NH3 conversion in neutral electrolyte because of big surface area, fast mass transport, superhydrophilic surface, and optimized electronic structure. B/Fe-Co2P HNCs can achieve the high NH3 yield rate (22.67 mg h−1 mgcat−1) as well as Faradaic efficiency (97.54%) for NO3−RR, greatly outperforming most of non-precious metal based NO3−RR electrocatalysts.
Cyclic polymers are a class of polymers that feature endless topology, and the synthesis of cyclic polymers has attracted the attention of many researchers. Herein, cyclic polymers were efficiently constructed by self-folding cyclization technique at high concentrations. Linear poly((oligo(ethylene glycol)acrylate)-co-(dodecyl acrylate)) (P(OEGA-co-DDA)) precursors with different ratios of hydrophilic and hydrophobic moieties were synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization using a bifunctional chain transfer agent with two anthryl end groups. The amphiphilic linear precursors underwent the self-folding process to generate polymeric nanoparticles in water. By irradiating the aqueous solution of the nanoparticles with 365 nm UV light, cyclic polymers were synthesized successfully via coupling of anthryl groups. The effects of the ratios of hydrophilic and hydrophobic moieties in linear P(OEGA-co-DDA) copolymers and polymer concentration on the purity of the obtained cyclic polymers were explored in detail via 1H nuclear magnetic resonance (1H NMR), dynamic light scattering (DLS), UV‒visible (vis) analysis, three-detection size exclusion chromatography (TD-SEC) and transmission electron microscopy (TEM). It was found that by adjusting the content of the hydrophilic segments in linear precursors, single chain polymeric nanoparticles (SCPNs) can be generated at high polymer concentrations. Therefore, cyclic polymers with high purity can be constructed efficiently. This method overcomes the limitation of traditional ring-closure method, which is typically conducted in highly dilute conditions, providing an efficient method for the scalable preparation of cyclic polymers.
Colorectal cancer causes the third most common type of malignant tumors with high morbidity and mortality. Chemotherapy is currently one of the most effective and common treatments for colorectal cancer. However, the poor water solubility of some chemotherapeutics, untargeted drug delivery, and the undesirable systemic side effects of conventional treatment remain the major issues for colorectal cancer chemotherapy. Fortunately, drug delivery systems (DDS) based on biomaterials have been widely investigated and found to be capable of resolving those issues with good performance. Therefore, the main goal of this review is to summarize and discuss the progress and potential advantages of different DDS for colorectal cancer chemotherapy. We not only reviewed the nanocarriers used to improve the solubility of chemotherapeutics, including liposomes, micelles, and nanoparticles, but also discussed targeted DDS based on specific ligand-receptor recognition and tumor microenvironmental stimulus responses. Furthermore, locally administered systems based on hydrogels and microspheres, which have been shown to increase drug accumulation at the tumor site while decreasing systemic toxicity, were also emphasized. DDS provides a good option for improving the efficacy of chemotherapy in the treatment of colorectal cancer.
Deoximation is an important transformation in synthetic industry. It can be employed in protection, characterization and purification of the carbonyls, and in the synthesis of ketones from non-carbonyl molecules. In the field, oxidative deoximation reaction can utilize the driving force caused by the oxidation process so that the reaction can occur under relatively mild conditions. Recently, we designed and prepared polyaniline-supported molybdenum (Mo@PANI) just by immersing PANI into the EtOH/H2O solution of MoCl5. The material was successfully applied as the efficient catalyst for oxidative deoximation reactions, which were performed in ethanol using H2O2 as the clean oxidant. The substrate scope of the reaction was wide. It could be applied on heterocycle-containing substrates, making this protocol preferable for pharmaceutical intermediate synthesis. Since Mo is a necessary trace element for both animals and plants, this method is environment-friendly and is suitable for large-scale preparation. This work as the first example of Mo-catalyzed oxidative deoximation reaction may inspire novel ideas for both catalyst design and synthetic process development.
The cubic S/N co-doped TiO2 (TNSx, x is the calcination temperature) photocatalysts with rich oxygen vacancies were obtained by high temperature calcination of sulfur powder and titanium-based MOFs NH2-MIL-125 for the photocatalytic removal of gaseous formaldehyde (a volatile organic compound). Among the obtained catalysts, the presence of oxygen vacancies restricted photogenerated electron and holes recombination. 98.00% removal of gaseous formaldehyde in 150 min could be achieved over TNS600 by xenon lamp. The removal efficiency for formaldehyde was well retained for five cycle experiment. The results from PL, TRPL and EIS revealed that TNS600 had the best separation efficiency of photogenerated electrons and holes, and the enhanced charge separation led to a significant increase in photocatalytic activity. The photocatalytic oxidation mechanism indicated that the •OH and •O2− radicals were mainly involved in the efficient elimination of gaseous formaldehyde and were able to mineralize formaldehyde to H2O and CO2.
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