Latest ArticlesThe design and synthesis of novel photocatalyst with self-temperature control function is an important topic in the field of advanced environmental functional materials. In this work, submicron-sized magnetic phase change microcapsules composed of paraffin core and Fe3O4-loaded silica shell are prepared, on which the Bi2WO6 crystals is grown in situ through hydrothermal reaction to obtain novel magnetic phase-change-microcapsule-supported Bi2WO6 catalyst (MP@FS/BWO). The MP@FS/BWO has a paraffin encapsulation ratio of 57.1%, and the phase change enthalpy of 105.1 J/g in a temperature range of 50–60 ℃, which endows the MP@FS/BWO with a certain self-temperature regulation ability. MP@FS/BWO shows excellent catalytic performance in the decomposition of rhodamine B under the simulated sunlight irradiation. After the light source is turned off, it still has good catalytic ability by maintaining high temperature due to its temperature control function based on the phase transition process. The MP@FS/BWO can be easily recycled by magnetic separation and shows good structural stability and reusability. This work provides a new idea for the development of long-effect and energy-saving outdoor photocatalysts.
Photothermal therapy (PTT) is a cutting-edge cancer treatment that can kill cancer cells in hypoxic environments without relying on oxygen. Seeking of the ideal photothermal agents with a high absorption coefficient in the near-infrared region, and a high excellent photothermal conversion efficiency is of great significance. Sulfone-Rhodanmine dye has showed an impressive absorption wavelength over 700 nm, but suffered from a stability issue. In this study, we synthesized five sulfone rhodamines and investigated the substitution effects on stability. SO2R2 showed high stability and strong absorbance at 714 nm with an excellent photothermal conversion efficiency of 53.06%, making it suitable for accurate photoacoustic imaging-guided photothermal therapy in vivo.
Luminescent materials that can be reversibly switched by electric field stimulation are attractive since the potential application for optoelectronic devices. Here we report a triplet-triplet annihilation upconversion (TTA-UC) system with electrophoretic response which is developed as the electrophoretic ink. The TTA-UC system consists of an ionic derivative of 9, 10-diphenyl anthracene (DPA) as the annihilator and Pt(Ⅱ) octaethylporphyrin (PtOEP) as the sensitizer. Upon applying an electric field, migration and enrichment of positively charged DPA derivatives towards the cathode results in a 20% enhancement of TTA-UC. A quasi-solid film for electrically writing is made using the electrophoretic TTA system as the ink and a platinum electrode as a pen. The prototype of TTA-UC ink demonstrates unique luminescence functions upon electrically writing and erasing, providing a promising strategy to develop electronic devices for display, information storage and encryption.
Vanadium flow batteries (VFBs) have drawn considerable attention as an emerging technology for large-scale energy storage systems (ESSs). One of the pivotal challenges is the availability of eligible ion exchange membranes (ICMs) that provide high ion selectivity, proton conductivity, and stability under rigorous condition. Herein, a 'side-chain-type' strategy has been employed to fabricate highly stable phenolphthalein-based cardo poly(arylene ether ketone)s (PAEKs) membrane with low area resistance (0.058 Ω cm2), in which flexible alkyl spacers effectively alleviated inductive withdrawing effect from terminal ion exchange groups thus enabling a stable backbone. The assembled VFBs based on PAEKs bearing pendent alkyl chain terminated with quaternary ammonium (Q-PPhEK) demonstrated an energy efficiency above 80% over 700 cycles at 160 mA/cm2. Such a remarkable results revealed that the side-chain-type strategy contributed to enhancing the ICMs stability in strong oxidizing environment, meanwhile, more interesting backbones would be woken with this design engaging in stable ICMs for VFBs.
In 2022, The MOE Key Laboratory of Macromolecular Synthesis and Functionalization in Zhejiang University had achieved several important results. First, a series of well-defined dinuclear organoboron catalysts were developed to precisely control the enchainment of ether and carbonate segments during the copolymerization of CO2 and epoxides. Second, polyester had been synthesized through cationic copolymerization of cyclic anhydride. Third, ring-opening polymerization of carbon dioxide based valerolactone had been achieved, revealing the prospect of 3-ethylidene-6-vinyltetrahydro-2H-pyran-2-one (EVL) in utilizing CO2 and synthesizing functional polymers. Fourth, machine learning methods have been applied to biomaterial research, enabling high-throughput screening of functional biomaterial surfaces for implantable devices, and searching for potent antimicrobial peptides in whole combinatorial peptide libraries. Fifth, methods of characterization of biomacromolecule RNA transcription and manipulation of nucleoside modification were developed. Sixth, artificial enzymes-armed Bifidobacterium Longum probiotics were established to tune down gut inflammation. Seventh, three-dimensional (3D) printing technologies were used to engineer tough supramolecular hydrogels. Eighth, hydroplastic foaming graphene frameworks for acoustic and conductive polymer composites were provided for application. Ninth, aggregate photophysics about the nature of through-space interactions (TSIs) and manipulating their strength in small molecules with non-conjugated structure had been elucidated. Tenth, the forming mechanism of a newfound nested texture in poly(l-lactic acid) (PLLA) spherulitic films had been revealed. Finally, the isotropically dyeing mechanism of KDP single crystals grown from hydrogels have been explored. The related works are reviewed in this paper.
A new continuous-flow process for the enzymatic synthesis of optically pure γ-lactones, which are used as flavors and fragrances in the food and cosmetic industries, was developed in a three-dimensional microfluidic reactor. The microchannels (175 mm in length, 0.9 mm in depth, and 1.72 mL in volume) were carved precisely inside a single borosilicate glass (90 mm × 75 mm × 12 mm) with ultrafast femtosecond laser micromachining. The flow field analysis and reaction simulation showed that the mixing of substrates and enzymes was enhanced, allowing the adjustment of residence time in a wide window. SmCRV4, a carbonyl reductase with excellent catalytic activity and enantioselectivity toward γ/δ-keto acids, was employed for the asymmetric synthesis of various chiral lactones. 30 mmol/L (R)-γ-decalactone (3g) can be obtained in 26 s with a space-time yield (STY) up to 16,877 g L−1 d−1, which is 14.4 times higher than the highest STY of batch reaction reported previously. This continuous-flow process was applied to the synthesis of 6 chiral lactones. In addition, the scaled-up synthesis of 3g was carried out in 6 cascade microreactors continuously for 6 h, demonstrating the feasibility and stability of the 3D continuous-flow process in enzymatic synthesis of optically pure compounds.
Molecular sieve catalysts, owing to their unique chemical properties, are widely used as catalysts among various catalytic reactions. Abundant Brønsted acid sites in molecular sieve catalysts usually enable active components to disperse well on the catalyst surface, and help to adsorb a large number of gas molecules to achieve maximum catalytic performance. Therefore, a variety of molecular sieve catalysts have been developed and used in the selective catalytic reduction of NOx by NH3 (NH3-SCR). For example, Cu molecular sieve catalysts such as Cu-SSZ-13 and Cu-SAPO-34 with wide temperature windows and stable structure are considered and applied as commercial catalysts for NOx removal in diesel vehicles for a long time. Although molecular sieve catalysts possess many advantages, they still cannot avoid the serious deactivation caused by various factors in practical applications. In this review, reasons leading to the deactivation of molecular sieve catalysts for NOx reduction in actual working conditions were concluded. The deactivation mechanisms of molecular sieve catalysts for NOx reduction were analyzed and the corresponding anti-deactivation strategies were summarized. Finally, challenges and prospects of molecular sieve catalysts for NOx reduction were also proposed.
Matrix-assisted laser desorption/ionization (MALDI) mass spectrometry (MS) plays an indispensable role in analyzing protein covalent structures. The reliable identification of amino acid residues and modifications relies on the mass accuracy, which is highly dependent on calibration. However, the accuracy provided by the currently available calibrants still needs further improvement in terms of compatibility with multiple tandem MS modes or ion polarity modes, calibratable range, and minimizing suppression of and interference with analyte signals. Here aiming at developing a versatile calibrant to solve these problem, we designed a synthetic peptide format of calibrant R(GDP) (referred to as "Gly-Asp-Pro, GDP") according to the chemical natures of amino acids and polypeptide fragmentation rules in tandem MS. With four types of amino acid residues selected and arranged through rational designs, a GDP peptide produces highly regulated fragments that give rise to evenly spaced signals in each tandem MS mode and is compatible with both positive and negative ion modes. In internal calibration, its regulated fragmentation pattern minimizes interference with analyte signals, and using a single peptide as the input minimizes suppression of the analyte signals. As demonstrated by analyses of proteins including monoclonal antibody and Aβ-42, these features allowed significant increase of the mass accuracy and precision, which improved sequence coverage and sequence resolution in sequence analyses (including de novo sequencing). This rational design strategy may also inspire further development of synthetic calibrants that benefit structural analysis of biomolecules.
Small-molecule drugs are widely used in daily life. There are still issues with the current industrial synthesis techniques for small-molecule drugs, such as the use of expensive metal catalysts, convoluted reaction processes, and non-recyclable catalysts. The benefits of photocatalytic organic synthesis over conventional techniques are mild conditions, environmental friendliness, and great selectivity. Porous framework materials can precisely modulate catalytic sites’ electronic state and ligand structure to improve photocatalytic performance. In particular, MOFs, COFs and PCCs based photocatalysts have received extensive research interest due to their unique morphology, structural adjustability, high photocatalytic performance, unique recyclability, excellent chemical stability, easy synthesis and low cost. Therefore, a key area for future research is the development of porous framework materials as photocatalysts for the synthesis of small-molecule drugs or drug precursors.
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