Latest ArticlesThe design and syntheses of metal-organic cages (MOCs) based on polyoxometalates (POMs) building blocks have attracted increasing attention due to their intriguing molecular architectures and physicochemical properties. In this work, we have successfully synthesized and systematically characterized a tetrahedral polyoxometalate-based organic cage (POC), K3Na17H12[(C4H6O6)6[Ni4(OH)3(A-α-SiW9O34)]4]·96H2O (Ni16L6(SiW9)4), using tritopic Ni4-substituted Keggin cluster (Ni4SiW9) as nodes and flexible L-(+)-tartaric acid ligands as linkers. The resulting POC tetrahedron has been firstly investigated as efficient catalyst for visible-light-driven hydrogen production, achieving a turnover number of 15,500 after 96-h photocatalysis. Such high catalytic performance of Ni16L6(SiW9)4 POC catalyst could be attributed to its unique cage structure, thereby offering more efficient catalytic component accessibility. In addition, spectroscopic analyses illustrated the photocatalytic mechanism and the structural stability of the TBA-Ni16L6(SiW9)4 catalyst during the photocatalytic process.
Pretreatment of the carrier for supported catalysts can effectively improve the strong metal-support interaction (SMSI) and increase the dispersion of precious metals, which are critical to many important catalytic reactions. In this work, we tuned SMSI on Pd/TiO2 catalysts through inducing surface defects of TiO2 by pretreated with different atmospheres (H2/N2, N2, O2/N2) at the high temperature (800 ℃). Multiple characterization results illustrated that surface defects anchored Pd species and thus enhanced their dispersion. During reduction, Ti3+ species formed and transferred onto the metallic Pd species and then induced SMSI, which effectively stabilize Pd species in the metallic state. The stronger MSI, the more stability of Pd species. As a case, Pd/TiO2–800H2, with strongest MSI, displayed the best HCHO oxidation performance at low temperature (10 ℃).
The application of photothermal therapy (PTT) is greatly limited by the low accumulation of photothermal agents, uneven photothermal distribution, and heat endurance of cancer cells. Worse still, despite PTT enhances immunogenicity, the anti-tumor immune efficacy is still unsatisfactory due to the inefficient immunogenic cell death (ICD) induction and poor infiltration of immune cells. To solve the above problems of PTT, we developed hyaluronic acid (HA) modified hollow copper sulfide nanoparticles encapsulating diethyldithiocarbamate (DDTC) to construct a breast tumor targeting and near infrared (NIR) photo-responsive drug delivery system (D-HCuS@HA), which further combined with losartan to improve the accumulation and penetration in the tumor site. Upon irradiation, D-HCuS@HA realized enhanced PTT and released cytotoxic Cu(DDTC)2 to eliminate heat endurance tumor cells, thereby enhancing anti-tumor effect and inducing effective ICD. Moreover, the combination with losartan could remodel the tumor microenvironment, allowing more T cells to infiltrate into the tumor, and significantly inhibiting the occurrence and development of metastatic tumors. In vitro/vivo results revealed the great potential of D-HCuS@HA combined with losartan, which provides a new paradigm for anti-tumor and anti-metastases.
Nitrene transfer reactions are powerful tools in synthetic organic chemistry. In recent years, transition-metal catalyzed nitrene transfer reactions with carbamates as the nitrene precursors have been widely pursued. Such species undergoes facile C−H amination, aziridination, and bifunctionalization of alkenes under the catalysis of different transition metals including Rh, Fe, Ru and others, enabling the efficient construction of various nitrogen-containing molecules. In this review, the recent developments in nitrene transfer reactions with carbamates via N−O bond cleavage were introduced based on different types of reaction, and the key mechanistic information and synthetic applications of the methodologies were discussed.
Nitrogen oxide (NOx) is one of the most critical contaminants in the air, and the control of NOx emission from diesel vehicles is very important. Cu-based small-pore zeolites have already been applied for NOx abatement on diesel vehicles. Among the small-pore zeolites, Cu-SSZ-50 catalysts with good NH3-SCR catalytic activity were believed to have potential for application. In this study, a one-pot synthesis method for Cu-SSZ-50 catalysts was developed for the first time, using the co-templates of Cu-TEPA and 2,6-dimethyl-N-methylpyridinium hydroxide. In this synthesis method, Cu-SSZ-50 with various Cu contents can be obtained by adjusting the amount of Cu-TEPA without the need for a further after-treatment process. The addition of Cu-TEPA affected the framework atoms and Cu species, and a lower Si/Al ratio and more SCR active Cu species were obtained. The synthesized catalyst with a Cu/Al ratio of 0.40 exhibited over 90% NOx conversion between 200 ℃ and 450 ℃ for the selective catalytic reduction of NOx with NH3 (NH3-SCR). Meanwhile, over 80% NOx conversion could be obtained from 250 ℃ to 450 ℃ after hydrothermal aging at 750 ℃ for 16 h. In addition, both L-H and E-R mechanisms were proven to exist for the one-pot-synthesized Cu-SSZ-50 by in situ DRIFTS experiments. The simple synthesis procedure, excellent catalytic activity and hydrothermal stability brighten the prospects for the application of Cu-SSZ-50.
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.
Polymerase chain reactions (PCR) are a very important tool for use in cloning, nucleic acid sequencing and diagnostic testing. The storage conditions of PCR reagents are limited to freezing and a lot of mixing steps are needed. In this paper, we report using metal ions to form coordination nanomaterials with the intrinsic components of the PCR reagents including dNTP, DNA primers and DNA polymerase as an integrated PCR reaction system. To complete PCR reactions, users need only to dissolve the coordination nanomaterials with a buffer and add template DNA. A few transition metal ions were screened and Cu2+ was found to be the most effective metal ion for this purpose. Then the encapsulation efficiency of PCR reagents was measured, which can reach close to 100% for the primers and DNA polymerase, but only 10% for dNTP because dNTP was excess. Further study also exhibited this integrated PCR reaction system can be used for DNA detection with a similar detection limit to the normal PCR, and showed good stability of encapsulated PCR nanomaterial after storage for a week.
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.
Introducing covalently crosslinked network to polymer matrix can merge the advantages in reprocessing and durability of polymers. In this contribution, a series of high-performance vitrimeric elastomers were achieved via polycondensation. The topological structures of polymers were tuned by varying the feeding ratios of bisacetoacetate, hex–substituted bisacetoacetate, bisamine and tris(2-aminoethyl)amine. With these structural manipulations, the vitrimeric elastomers presented great elastic recovery properties (strain recovery value up to 80%) benefiting from the introduction of long chain branch. Furthermore, the elastomers exhibited excellent reprocessing property, water vapor/oxygen barrier and adhesive properties. Specially, the elastomers could be degraded into monomer under acid conditions which enabled the elastomer synthesis again in closed loop recycling system. The ease of the polycondensation in this work to prepare highly elastic and recyclable vitrimeric elastomers demonstrated exciting opportunities for the synthesis of sustainable polymers.
The pharmaceutical industry is now paying increased attention to continuous manufacturing. While the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world, the advancement of automated pharmaceutical continuous manufacturing in China is relatively slow due to some key challenges including the lack of knowledge on the related technologies and shortage of qualified personnels. In this review, emphasis is given to two of the crucial technologies in automated pharmaceutical continuous manufacturing, i.e., process analytical technology (PAT) and self-optimizing algorithm. Research work published in recent 5 years employing advanced PAT tools and self-optimization algorithms is introduced, which represents the great progress that has been made in automated pharmaceutical continuous manufacturing.
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