Latest ArticlesThe development of core-shell nanoclusters with controllable composition is of utmost importance as the material properties depend on their constituent elements. However, precisely tuning their compositions at the atomic scale is not easily achieved because of the difficulty of using limited macroscopic synthetic methods for atomic-level modulation. In this work, we report an interesting example of precisely regulating the core composition of an inorganic core-shell-type cobalt polyoxoniobate [Co26Nb36O140]32− by controlling reaction conditions, in which the inner Co-core composition could be tune while retaining the outer Nb-shell composition of resulting product, leading to a series of isostructural species with a general formula of {Co26-nNb36+nO140} (n = 0–2). These rare species not only can display good powder and single-crystal proton conductivities, but also might provide helpful and atomic-level insights into the syntheses, structures and composition modifications of inorganic amorphous core-shell heterometal oxide nanoparticles.
Sequential energy transfer is ubiquitous in natural light-harvesting systems (LHSs), which greatly promotes the exploitation of light energy. The LHSs in nature are sophisticated supramolecular assemblies of chlorophyll molecules that carry out efficient light harvesting through cascade energy transfer process. Inspired by nature, scientists have paid much attention to fabricate stepwise LHSs based on assorted supramolecular scaffolds in recent years. Light-harvesting antennas and energy acceptors can be accommodated in particular scaffolds, which offer great convenience for energy transfer between them. These systems not only further mimic photosynthesis, but also demonstrate many potential applications, such as photocatalysis, tunable luminescence, and information encryption, etc. In this review article, aiming at offering a practical guide to this emerging research field, the introduction of construction strategies towards sequential LHSs will be presented. Different scaffolds are classified and highlighted, including host-guest assemblies, metal-coordination assemblies, as well as bio-macromolecular and other supramolecular scaffolds.
A sustainable and practical process is presented for the direct synthesis of sodium tanshinone IIA sulfonate (STS). Our approach was inspired by the well-established and industrially applied batch synthetic route for STS production. We constructed a telescoped two-step continuous flow platform. This involved a continuous tanshinone IIA sulfonation and in-line salt formation. For the setup, we constructed a 3D circular cyclone-type microreactor using femtosecond laser micromachining. Compared to the 68% yield for 2 h in batch, the two-step continuous flow had an STS yield of 90%, achieved for a total residence time of < 3.0 min under optimal conditions. The proposed continuous flow method vastly simplified the operation and improved procedural safety, while significantly reducing the required acid content and wastewater production.
Pillar[n]arenes are a novel class of macrocyclic hosts reported by Ogoshi and co-workers in 2008. Because of their rigid pillar structures, interesting host–guest properties and ease of modifications, pillar[n]arenes have been developed rapidly in the field of functional materials and biomedicine. The modifications of pillar[n]arenes at different positions can give them varied characteristics. Functional groups can be introduced into one position of pillar[n]arenes without changing host–guest properties of pillar[n]arenes. A series of pillar[n]arene dimers, trimers, tetramers and metallacycles can be constructed by mono-functionalized pillar[n]arenes. In this review, two synthetic methods of mono-functionalized pillar[n]arenes are summarized and structures containing mono-functionalized pillar[n]arenes are described. Furthermore, the applications of mono-functionalized pillar[n]arenes in different fields (e.g., supramolecular polymers, sensors, molecular machines, catalysis, biological applications and light-harvesting systems) are also introduced. Hopefully, this article will be useful for researchers studying pillar[n]arenes, especially the mono-functionalized pillar[n]arenes.
The recent advances in accelerated polymerization of N-carboxyanhydrides (NCAs) offer an effective strategy to simplify the preparation of polypeptide materials. However, the fine-tuning of polymerization kinetics, which is critical to differentiate the main polymerization and the side reactions, remains largely unexplored. Herein we report the modulation of polymerization rate of NCA in a water/oil biphasic system. By altering the aqueous pH, the initial location of the initiators, and the pKa of initiating amines, we observed the change in polymerization time from several minutes to a few hours. Due to the high interfacial activity and low pKa value, controlled polymerization was observed from multi-amine initiators even if they were initially located in the aqueous phase. This work not only improves our understanding on the biphasic polymerization mechanism, but also facilitates preparation of versatile polypeptide materials.
The development of n-type semiconductor is still far behind that of p-type semiconductor on account of the challenges in enhancing carrier mobility and environmental stability. Herein, by blending with the polymers, n-type ultrathin crystalline thin film was successfully prepared by the method of meniscus-guided coating. Remarkably, the n-type crystalline films exhibit ultrathin thickness as low as 5 nm and excellent mobility of 1.58 cm2 V−1 s−1, which is outstanding in currently reported organic n-type transistors. Moreover, the PS layer provides a high-quality interface with ultralow defect which has strong resistance to external interference with excellent long-term stability, paving the way for the application of n-type transistors in logic circuits.
Early diagnosis and treatment of cancer requires the development of tools that are both sensitive and selective in detecting spermine. In this study, we presented a "supramolecular cyclization-induced emission enhancement" strategy for the sensitive and selective detection of spermine. A new pillar[5]arene probe (P1) demonstrated excellent solution/solid dual-state emission properties, and the addition of certain spermine (Spm) resulted in fluorescence enhancement due to the synergy of multiple weak interactions that restricted the free motion of P1 in the P1⊃Spm complex. This mechanism was further confirmed by time-resolved spectroscopy, DFT calculations, and IGM analysis. With its low limit of detection and high selectivity, P1 is a promising tool for measuring spermine in artificial urine samples.
Photodynamic therapy (PDT) is a clinically approved cancer treatment that uses energy of light to generate active substances that cause damage to the cancer. Photosensitizers are employed to absorb light and generate toxic reactive oxygen species (ROS) to damage biomolecules like DNA. At the same time, some chemotherapy drugs like nucleotide analogues can provide mechanism-guided promotion in the treatment efficacy of PDT. However, the photosensitizer and chemotherapy drugs used in PDT is usually organic molecules, which suffers from bad solubility, fast clearance, and acute toxicity. To achieve targeted treatment, a reasonable delivery system is necessary. Therefore, we reported a metal-phenolic network where IR780 and gemcitabine were coupled chemically to overcome these shortcomings. The enhanced PDT effects can be realized by the promoted cell death both in vitro and in vivo. Moreover, the synergistic therapy also induced T-cell mediated anti-tumor immune response, which was significant for the inhibition of distant tumor growth. This work expanded the biomedical application of metal-phenolic materials and contribute to the wider application of photodynamic cancer therapy.
Electrosynthesis of hydrogen peroxide (H2O2) is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features. The crucial point remains developing highly active, selective and cost-effective electrocatalysts. The electrosynthesis of H2O2 in acidic media is more practical owing to its stability and no need for further purification. We herein report a phosphorus and selenium tuning Co-based non-precious catalyst (CoPSe) toward two-electron oxygen reduction reaction (2e– ORR) to produce H2O2 in acidic media. The starting point of using both P and Se is finding a balance between strong ORR activity of CoSe and weak activity of CoP. The results demonstrated that the CoPSe catalyst exhibited the optimized 2e– ORR activity compared with CoP and CoSe. It disclosed an onset potential of 0.68 V and the H2O2 selectivity 76%-85% in a wide potential range (0–0.5 V). Notably, the CoPSe catalyst overcomes a significant challenge of a narrow-range selectivity for transition-metal based 2e– ORR catalysts. Finally, combining with electro-Fenton reaction, an on-site system was constructed for efficient degradation of organic pollutants. This work provides a promising non-precious Co-based electrocatalyst for the electrosynthesis of H2O2 in acidic media.
In this study, magnesium and coconut shell carbon (CSC) were prepared by a ball milled process and used for water disinfection with adsorbing tiny amounts of copper(Ⅱ). Dissolved oxygen (DO) was reduced to hydrogen peroxide (H2O2) via a two-electron pathway by Mg corrosion. Cu(Ⅱ) in the wastewater will be enriched on the CSC surface and efficiently catalyzes H2O2 for inactivating E. coli. The results show that E. coli with an initial concentration of approximately 106 CFU/mL was under the detection limit (< 4 CFU/mL) within 15 min. All of the Cu(Ⅱ) could be adsorbed by the composite and catalyzed H2O2 to different active species. The quenching experiments, electron spin resonance (ESR) capture measurements and the UV-vis spectroscopy detection confirmed the present of the hydroxyl radicals (•OH), superoxide radicals (•O2−) and Cu(Ⅲ). Different with tradition Fenton like process, Cu(Ⅲ), rather than radicals, played the major role during the Mg-CSC/Cu(Ⅱ) process. In addition to the cellular membrane damage, most of the bacterial genomic DNA was also be degraded and the bacterial reactivation was avoided. The Mg-CSC/Cu(Ⅱ) process also showed a satisfied disinfection performance in real wastewater treatment. Overall, this study provides a new strategy for water disinfection.
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