Latest ArticlesThe synthesis of degradable polymers with easy-to-break in-chain carbon-oxygen bonds has attracted much attention. This minireview introduces the synthesis of a variety of degradable polymers from the (co)polymerizations of several typical oxygenated monomers such as epoxides, cyclic carbonates, cyclic esters, carbon dioxide (CO2), carbonyl sulfide (COS), and cyclic anhydrides. We highlight the catalysts and mechanisms for these (co)polymerizations. The ring-opening copolymerization of five-membered carbonate with cyclic anhydride or COS has been introduced. We also highlight the synthesis of block copolymers and cyclic copolymers with well-defined sequences by the method of growing center switching. We hope that these new polymerization systems can provide new ideas for the development of degradable low-carbon polymers in the future.
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.
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.
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.
A new strategy to induce vesicle fusion has been developed by employing pillar[5]arene derivatives that were channel-like and were prepared by appending side chains onto pillar[5]arenes backbones. The channels feature with hydrophilic negatively and positively charged groups at both ends and hydrophobic Trp residues at the outer surface, which endows the channels with amphiphilicity. The zwitterionic amphiphilic channels could spontaneously incorporate into the bilayer membranes of lipid vesicles to induce vesicle fusion driven by the electrostatic interactions between negatively charged and positively charged groups.
Molecular doping has become a widely used method to modulate the electric performance of organic semiconductors (OSC). Highly effective charge transfer during molecular doping is desired to achieve ideal electrical conductivity. Two types of charge transfer mechanisms are widely accepted in molecular doping process: integer charge transfer (ICT) and charge transfer complex (CTC). In this review, fundamental principles of two mechanisms are revisited and the characterization methods are depicted. The key points for the formation of two mechanisms are highlighted from aspects of molecular structure and process engineering. Then, the strategies to improve the proportion of ICT are discussed. Finally, the challenges and perspectives for future developments in the molecular doping of polymer semiconductors are provided.
Photothermal effect has been widely employed in the H2 evolution process at the advantage of using clean energy sources to produce another one of higher benefits. The solar-to-heat conversion have various forms and heat can facilitate reactions in a variety of dimensions. Hence, summarizing the sources and destinations of heat is important for constructing hydrogen production systems of higher efficiency. This view mainly focuses on the recent state-of-art progress of hydrogen evolution reaction (HER) based on photothermal effect. First, we introduce the main pathways of photothermal conversions applied in H2 evolution. Then, the functions of the photothermal effect are clearly summarized. Furthermore, we go beyond the catalytic reaction and introduce a method to improve the catalytic system by changing the catalytic bulk phase through thermal means. In the end, we sort out the challenges and outlook to offer some noble insights for this promising area.
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.
The development of molecular probes or systems with the ability of multiple orthogonal responses is an effective approach to precisely detect biomolecules with similar chemical structures. Herein, we report the synthesis of a water-soluble TPE-based octacationic cage (1) with the compressed TPE-containing bilayer, which endows it with good fluorescence properties and potential conformation chirality. As a result, 1 exhibits molecular recognition for anionic nucleotides within its two “claw”-like cavities to form 1:2 host-guest complexes in water, companying with selective turn-off fluorescence and turn-on CD responses to G/GTP over other nucleotides.
Increasing environmental pollution and shortage of conventional fossil fuels have made it urgent to develop renewable and clean energy sources. Electrocatalytic water splitting, with its abundant raw materials, simple process, and zero carbon emission, is considered one of the most promising processes for producing carbon-neutral hydrogen which has excellent energy conversion efficiency and high gravimetric energy density. Among them, oxygen evolution reaction (OER) electrocatalysts and hydrogen evolution reaction (HER) electrocatalysts are critical to decreasing the intrinsic reaction energy barrier and boosting the hydrogen evolution efficiency. Therefore, it is imperative to develop and design low-cost, highly active, and stable OER and HER electrocatalysts to lower the overpotential and drive the electrocatalytic reactions. Transition metal sulfides, especially iron-based sulfides, have attracted extensive exploration by researchers as a result of its high abundance in the Earth's crust and near-metallic conductivity. Consequently, in this review, we systematically and comprehensively summarize the progress in the application of iron-based sulfides and their composites as OER and HER electrocatalysts in electrocatalysis. Detailed descriptions and illustrations of the special relationships among their composition, structure, and electrocatalytic performance are presented. Finally, this review points out the challenges and future prospects of iron-based sulfides in practical applications for designing and fabricating more promising iron-based sulfide OER and HER electrocatalysts. We believe that iron-based sulfide materials will have a wide range of application prospects as OER and HER electrocatalysts in the future.
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