Latest ArticlesPerpyrrospirone A (1) characterized an unprecedented 6/5/6/8/5/13/6 oxahexacyclic scaffold with a unique peroxide-bridged 8, 9-dioxa-2-azaspiro[4.7]dodecane core from marine-derived Penicillium citrinum. Compounds 2 and 3 possessed rare oxatetracyclic (6/5/6/5) skeleton fused with a 13-menbered-ring macrocyclic moiety. Their structure and absolute configurations were determined by comprehensive spectroscopic analyses, ECD data coupled with TD-DFT calculations and X-ray diffraction experiments. In addition, 7 showed cytotoxicity and induced apoptosis of Hela cells in a dose-dependent manner after a 48 h treatment.
Many previous studies have shown that the molecular structures of oligothiophene derivatives including molecular skeleton and alkyl chains have a significant effect on their self-assemblies on the surface. In this work, a series of linear oligothiophene derivatives (DCV-nT-Hex, n = 3~11) modified with terminal dicyanovinyls and alkyl chains were adopted to further investigate the different assembly behaviors at liquid-solid interface by scanning tunneling microscopy (STM). Interestingly, via the hydrogen bonding and van der Waals interactions, DCV-3T-Hex formed zigzag and flower structures while DCV-nT-Hex (n = 4~11) formed lamellar structures. Density functional theory (DFT) calculations show that for the most energetically favorable configurations of DCV-nT-Hex, the different distribution of alkyl chains affected intermolecular interactions, and ultimately led to the different assembled structures. The zigzag and flower structures of DCV-3T-Hex had preferential thermodynamic stability compared to other structures of DCV-nT-Hex (n = 4~11). In addition, self-assembled nanostructures of DCV-nT-Hex molecules with even numbers (n = 4, 6, 8, 10) were overall more stable than those with odd numbers (n = 5, 7, 9, 11), and the stability of the self-assembled structure was weakened with the extension of the molecular backbone, individually. The orientation of molecular alkyl chains was found to greatly affect the intermolecular interactions and thus leading to various self-assembly structures of DCV-nT-Hex (n = 3~11).
Click chemistry has become a useful tool for diverse molecular linkage and modification, and the development of new click strategy that enable reversibility and multifunctionality is of high demand for the multifunction and drug release. Herein, compositionally clicking combined regioselective iridium-catalyzed azide-alkynthio cycloaddition (Ir-AAC) and disulfuration has been developed for the sequential linkage from N-acetylenethio phthalimides, naturally occurring thiols and readily available azides. This method has been successfully applied to the construction of drug hybrids, peptide modification and glycosylation. Furthermore, by the design of diacetylenethio phthalimide as a platform molecule, trifunctional conjugants were sequentially linked through independent Ir-AAC, disulfuration and Cu-AAC reaction for hydrophobic tagging ternary PROTACs.
To realize the handedness controllable circularly polarized luminescence (CPL) system remains challenging. Herein, the solvent-mediated CPL inversion and amplification systems were successfully constructed by camptothecin derivative (CPT-A). Due to the planar structure of N, N-dimethylformamide, it could co-assemble with CPT-A, resulting in the alteration of glum from ‒0.0082 to +0.0085 by increasing water content. While in the non-planar solvent (hexafluoroisopropanol), the glum was amplified to 0.034 with the increase in water content. Moreover, the CPT-A could react with the glutathione, resulting in the anticancer drug CPT to make it more toxic to the cancer cells. Overall, the handedness controllable CPL systems were realized by tuning the supramolecular self-assembly of a prodrug.
Li metal has been regarded as the holy grail for the next-generation Li-ion battery. Li dendrites issues, however, impede its practical application. In general, prolonging the sand time of Li nucleation and regulating homogeneous Li+ flux are effective approaches to suppress the dendrites formation and growth. Regarding this view, a functional polypropylene (PP) separator is developed to regulate ion transportation via a newly designed Li-based metal-organic framework (Li-MOF) coating. The Li-MOF crystallizes in the orthorhombic space group P212121 and features a double-walled three-dimensional (3D) structure with 1D channels. The well-defined intrinsic nanochannels of Li-MOF and the steric-hinerance effect both restrict free migration of anions, contributing to a high Li+ transference number of 0.65, which improve the Sand time of Li nucleation. Meanwhile, the Li-MOF coating with uniform porous structure promotes homogeneous Li+ flux at the surface of Li metal. Furthermore, the Li-MOF coating layer helps to build solid-electrolyte interphase (SEI) layer that comprises of inorganic LiF and Li3N, which further prohibits the dendrites growth. Consequently, a highly stable Li plating/stripping cycling for over 1000 h is achieved. The functional separator also enables high-performance full lithium metal cells, the high-rate and long-stable cycling performance of LiNi0.8Mn0.1Co0.1 (NMC811)-Li and LiCoO2 (LCO)-Li cells further demonstrate the feasibility of this concept.
A novel metabolic chemical reporter of Ac36deoGlcNAz was developed and confirmed as an effective probe for O-GlcNAc modification. Ac36deoGlcNAz labeling predominantly occurs in intracellular O-GlcNAcylated proteins rather than cell-surface glycoproteins. Of note, it could reduce the artificial S-glyco-modification compared to Ac4GalNAz and Ac4GlcNAz. This new reporter allows to be widely used in the field of proteomic identification of O-GlcNAcylation.
A facile and environmentally friendly visible-light-induced three-component reaction of α-diazoesters, cyclic ethers and NaSCN to construct organic thiocyanates has been developed at room temperature. This reaction could occur under photocatalyst- and additive-free conditions to afford a number of organic thiocyanates with moderate to good yield and favorable functional group tolerance.
A Cu-catalyzed chemoselective heterocyclization of o-cinnamoyl arylisocyanides with α-substituted tosylmethyl isocyanides is developed for the efficient synthesis benzopyrroloazepinones. An isocyanide insertion into the C–Cu bond of organocuprate intermediate is involved for the formation of the seven-membered azepinone ring.
Amyloid proteins correlate with a series of degenerative diseases. Targeting amyloid aggregation has remained a hot topic in therapeutic studies. Numerous inhibitors have been developed, but very few have been approved for marketing. Meanwhile, the growing knowledge of amyloid structural characteristics provides a basis for the rational design of inhibitors. Here we introduce the high-resolution structural findings of amyloid fibrils in recent years and discuss the reported strategies toward rationally designed inhibitors based on amyloid-related structural studies.
Aqueous zinc-ion batteries (AZIBs) have aroused significant research interest around the world in the past decade. The use of low-cost aqueous electrolytes and a metallic Zn anode with a suitable redox potential and high energy density make AZIBs a potential alternative to commercial Li-ion batteries in the development of next-generation batteries. However, owing to the narrow electrochemical stability window (ESW) of aqueous electrolytes, the choice of cathode materials is limited, because of which AZIBs exhibit a relatively low operating voltage and energy density. Hence, expanding the ESW of aqueous electrolytes is important for the development of practical AZIBs. This paper systematically reviews the electrolyte engineering strategies being explored to broaden the ESW of AZIBs. An in-depth analysis of high-voltage AZIBs is also presented. We suggest that the realization of high-voltage AZIBs depends on the synergistic development of suitable electrolytes and cathode materials. In addition, the cost associated with their fabrication as well as the use of standardized electrochemical tests should be considered during the design of high-voltage AZIBs.
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