Latest ArticlesThe rapid and precise fabrication of multiscale supramolecular assemblies using micro/nanofluidic techniques has emerged as a dynamic area of research in supramolecular chemistry, materials chemistry, and organic chemistry. This review summarizes the application of micro/nanofluidic techniques in constructing supramolecular assemblies, including nanoscale supramolecular assemblies such as macrocycles and cages, microscale supramolecular assemblies such as metal organic frameworks (MOFs) and covalent organic frameworks (COFs), and macroscale supramolecular assemblies such as supramolecular hydrogels. Compared to conventional synthesis methods, micro/nanofluidic techniques for the production of supramolecular assemblies have significant advantages, including enhanced safety, high reaction rates, improved selectivity/yield, and scalability. Additionally, micro/nanofluidic systems facilitate the creation of precisely controllable micro/nanoconfined environments, allowing for a unique flow behavior that improves our understanding of the supramolecular self-assembly process. Such systems may also lead to the development of novel supramolecular assemblies that differ from those generated via traditional methods.
Hospital sewage contains various harmful pharmaceutical contaminants (e.g., antibiotics, anti-inflammatory agents, and painkillers) and pathogens (e.g., bacteria, viruses, and parasites), whose direct discharge into the environment will induce diseases and pose a powerful threat to human health and safety, and environmental ecology. In recent years, advanced oxidation processes (AOPs), particularly photocatalysis, electrocatalysis, and ozone catalysis have been developed as widespread and effective techniques for hospital sewage treatments. However, there is a lack of systematic comparison and review of the prior studies on hospital sewage treatment using AOPs systems. This review elaborates on the mechanisms, removal efficiencies, and advantages/disadvantages of these AOPs systems for hospital wastewater decontamination and disinfection. Meanwhile, some novel and potential technologies such as photo-electrocatalysis, electro-peroxone, Fenton/Fenton-like, and piezoelectric catalysis are also included and summarized. Moreover, we further summarize and compare the capacity of these AOPs to treat the actual hospital wastewater under the impact of the water matrix and pH, and estimate the economic cost of these technologies for practical application. Finally, the future development directions of AOPs for hospital wastewater decontamination and disinfection have been prospected. Overall, this study provides a comparison and overview of these AOP systems in an attempt to raise extensive concerns about hospital wastewater decontamination and disinfection technologies and guide researchers to discover the future directions of technologies optimization, which would be a crucial step forward in the field of hospital sewage treatment.
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.
High monomer concentration is a requisite for engendering the aggregation-induced emssion (AIE) phenomenon as well as the formation of supramolecular polymers. Therefore, this is supposed to ensure the generation of AIE supramolecular polymers, wherein the monomer soluability takes effect. Nevertheless, parts of supramolecular monomers are considered as poessessing different soluability towards the same sovlent, through which the polymerzation process is thus hard to proceed. Interfacial polymerzation gets over the soluabilty restriction, providing a facile method for propelling the reaction of thesemonomers. Herein, we had prepared M1 containing tetraphenylethene (TPE) functionalized with two terpyridine derivatives, then making M1 dissolving in CHCl3 to give solutions. Cu2+ solutions were fabricated through dissolving CuCl2 into H2O. Towards mixing those solutions, AIE interfacial supramolecular polymers (AIEISPs) displaying green fluorescence were generated at the interface of two phases on the basis of metal-coordination between terpyridine and Cu2+. These AIEISPs were certificated to possess the stimuli-responsiveness, for which the excessive addition of tetrabutylammonium hydroxide would cause the structure destruction owing to the stronger bonding ability with Cu2+ than that of terpyridine. These fabricated AIEISPs had provided a new avenue to prepare AIE supramolecular polymers.
Four pillar[5]arene-based bicyclic compounds, so-called molecular universal joint (MUJ), were synthesized by incorporating a bisamide ring containing N, O, or S-heteroatom groups, which served as stimuli-responsive chiroptical molecular devices. The structure of MUJ was confirmed by 1H NMR spectra and single-crystal X-ray diffraction analysis, and their planar-chiral enantiomers were successfully separated. Chiroptical inversion behaviors from in to out configurations triggered by temperature, solvent, and guest complexation were investigated by circular dichroism spectra. Chiroptical inversion could be realized in the presence of adiponitrile in certain solvents due to the solvation effects on the side ring and the threading of the guest into the pillar[5]arene cavity. However, the stronger self-included interactions between the cavity and the inside ring of certain MUJs led to inhibition of the switching.
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.
Nucleophilic phosphine and amine catalyst-switched chemodivergent [4 + 1] and [3 + 3] annulations of allenyl imides and β,γ-enones have been developed, furnishing highly substituted 2-cyclopentenone and 2-pyranone derivatives in moderate to excellent yields. Two plausible reaction mechanisms involving two different ketene intermediates have been proposed to explain the observed chemoselectivity. Moreover, by virtue of the α,β-enone substructure of the [4 + 1] adducts, 1,3-dipolar cycloaddition of nitrile imines has been studied in one-pot to provide various fused pyrazoline derivatives.
A series of photoinduced palladium-catalyzed 1,3-diene-selective fluoroalkylamination derivatives was rationally synthesized based on diversity-oriented synthesis via cross coupling of 1,3-dienes, amines and fluoroalkyl iodides. The reaction featured good function group tolerance and a broad substrate scope, which could be extended to the late-stage modification of bioactive molecules. Bactericidal activity of all the compounds against Xanthomonas oryzae pv. oryzae (Xoo) was evaluated. Among them, compound E14 showed significant activity against Xanthomonas oryzae pv. oryzae (Xoo) with half maximal effective concentration (EC50) value of 6.61 µmol/mL. In pot experiments, the results showed that E14 could control rice bacterial blight with protective and curative efficiencies of 37.5% and 63.2% at 200 µg/mL, respectively. Additionally, a plausible mechanism for antibacterial behavior of E14 was proposed by electron microscopy, flow cytometry, reactive oxygen species detection, and biofilm assay. In current work, it can promote the development of photoinduced palladium-catalyzed 1,3-diene-selective fluoroalkyl amination compounds as prospective antibacterial agent bearing an intriguing mode of action.
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.
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