Latest ArticlesThe XCF3 groups (X = O, S, Se) play an increasingly important role in modern organic chemistry due to their unique electronegativity, lipophilic nature, metabolic stability, and bioavailability. Heterocyclic compounds are important scaffolds in many bioactive compounds and drugs. The incorporation of XCF3 groups into heterocyclic compounds can change their physicochemical and biological properties, which injects new vitality into the application of heterocyclic compounds in many fields such as organic chemistry, the pharmaceutical chemistry, and life sciences. In this paper, the recent progress in the synthesis of F3CX-containing heterocycles is reviewed, and the application scope and mechanism of some reactions are discussed.
LiMn2O4 (LMO) is the substance of choice for small and medium-sized energy storage materials in daily life. In this work, Li3InCl6 (LIC) is prepared on the surface of LiMn2O4 by hydrothermal method using InCl3 and LiCl as raw materials. This method stabilizes the LMO crystal structure by uniformly coating the LIC on the LMO surface and effectively maintains the morphology of LMO crystals during the cycling process. SEM and EDS analysis confirm the morphology and homogeneity of the synthesized material LIC on the LMO surface. The prepared material is put into a battery, and the charge-discharge test is carried out at 0.5 C and 1 C. The results show that the LIC surface-modified samples exhibit more than 6% higher cycling performance than the unmodified samples after long cycling.
Lanthanide coordinated multicolor fluorescent polymeric hydrogels (MFPHs) are quite promising for various applications because of their sharp fluorescence bands and high color purity. However, few attempts have been carried out to locally regulate their fluorescence switching or shape deforming behaviors, but such studies are very useful for patterned materials with disparate functions. Herein, the picolinate moieties that can sensitize Tb3+/Eu3+ luminescence via antenna effect were chemically introduced into interpenetrating double networks to produce a robust kind of lanthanide coordinated MFPHs. Upon varying the doping ratio of Tb3+/Eu3+, fluorescence colors of the obtained hydrogels were continuously regulated from green to orange and then red. Importantly, spatial fluorescence color control within the hydrogel matrix could be facilely realized by controlled diffusion of Tb3+/Eu3+ ions, producing a number of 2D hydrogel objects with local multicolor fluorescent patterns. Furthermore, the differential swelling capacities between the fluorescent patterned and non-fluorescent parts led to interesting 2D-to-3D shape deformation to give well-defined multicolor fluorescent 3D hydrogel configurations. Based on these results, bio-inspired synergistic color/shape changeable actuators were demonstrated. The present study provided a promising strategy to achieve the local fluorescence and shape control within lanthanide coordinated hydrogels, and is expected to be expanded for fabricating useful patterned materials with disparate functions.
Self-immolative linkers have been widely used to construct prodrugs to improve their efficacy and safety. In this study, we report the use of phenoxysilyl linker as a self-immolative unit to prepare antibody-drug conjugates (ADCs). Phenoxysily based ADC Ate-PPS-CA4 was prepared and its release was systematically investigated by mass spectrometry. Biological evaluation showed that Ate-PPS-CA4 displayed the ability to target delivery and self-immolative release the active payload CA4 on PD-L1 positive cells MDA-MB-231. As the same with its payload CA4, it could arrest the cell cycle to the G2/M phase and induced changes in cell morphology at the dose of its IC50. The development of this linker with novel drug release mechanisms will expand the methodology to construct ADCs, especially for non-internalizing ADCs by extracellular cleavage.
Polyoxometalates (POMs) have conducive properties such as controlled Brønsted and Lewis acidity, high thermal stability, nontoxic nature, tunable solubility, and less corrosiveness. POMs have been extensively applied in catalytic organic reactions and have an exciting prospect for industrial applications. This review summarized recent progress in the application of POMs as acid catalysts for various organic reactions including CC bond formation, CN bond formation, CO bond formation, heterocyclic synthesis reactions, cyanosilylation and hydrolysis reactions. Various POMs catalysts including heteropoly acids (HPAs) and cationic functionalized HPAs with Brønsted acidity, HPAs supported on non-precious metal support with Brønsted acidity (or both Brønsted and Lewis acidity), transition metal substituted POMs with Lewis acidity were applied in above reactions. This review attempts to provide up-to-date information about POMs acid-catalyzed organic reactions and propose future prospects.
Colorectal cancer (CRC) is a lethal malignancy with a high mortality rate due to its low immunogenicity, the strong immunosuppressive milieu and poor drug permeability. To overcome these obstacles, a cascade synergistic nanosystem (denoted as R837/ICG@Lip) was developed via self-assembly of heater indocyanine green (ICG) and toll-like receptor-7 agonist imiquimod (R837) into thermosensitive liposome for simultaneous induction of immunogenic cell death (ICD) and reversing of suppressive tumor microenvironment. The obtained nanoparticles exhibited NIR-triggered drug release, good photothermal conversion efficiency and phototoxicity towards CT26 colorectal cancer cells. In vivo results reveal that the R837/ICG@Lip could be effectively accumulated in CT26 subcutaneous tumors and the draining lymph nodes. More importantly, R837/ICG@Lip-mediated low-temperature photothermal therapy triggers ICD, promotes the maturation of host dendritic cells (DCs), and subsequently amplifies adaptive antitumor T-cell responses, resulting in 'Cold to Hot' transition. Besides directly affecting immune cells, the secretion of some immune-related cytokines further indirectly boosted anti-cancer immunity. After combining with the indoleamine 2, 3-dioxygenase (IDO) inhibitor, the systemic antitumor immune response was further augmented, achieving best tumor inhibition effects. Thus, low-temperature mediated photoimmunotherapy targeting multiple antitumor immune pathways boost synergistic antitumor immunity of tolerance tumors.
Protein self-labeling tags achieve selective fusion and labeling of target proteins through genetic coding technology, but require exogenous fluorescent probes with fluorogenicity for protein tag binding to have the performance of wash-free fluorescence imaging in live cells. In this paper, we reported a fluorogenic probe 1 capable of ratiometric fluorescence recognition of SNAP-tag proteins. In this probe, the O6-benzylguanine derivative of 3–hydroxy-1,8-naphthalimide underwent a selective covalent linkage reaction with SNAP-tag protein. The hydroxyl group on the naphthalimide fluorophore formed a hydrogen bond with the functional group near the protein cavity. The excited state proton transfer occurred after illumination, to obtain the ratio fluorescence signal from blue emission to red emission, realizing the wash-free fluorescence imaging of the target proteins.
Antimony-based materials are considered as promising anodes for potassium ion batteries due to their high theoretical capacity and low electrode potential. However, the aggregation and bulk expansion of Sb particles in cycling will cause capacity attenuation and poor rate performance. In this paper, Sb nanoplates were designed to be embedded in flexible porous N-dopped carbon nanofibers (Sb@PCNFs) by a simple electrospinning deposition (ESD) method. In this structural design, Sb nanoplates of high capacity were employed as active materials, N-dopped carbon nanofibers were used to improve conductivity and structural stability. The introduction of pore-forming agent enables the nanofibers to possess porous structure, thus buffering the huge volume change and promoting the transfer of electrolyte/ions. More importantly, the freestanding film can be directly used as a working electrode, reducing the redundancy in the battery and the cost. Benefitting from the favorable structure, the freestanding flexible Sb@PCNFs electrode shows excellent potassium storage performance with a capacity of 314 mAh/g after 2000 cycles at 500 mA/g. This strategy of employing active material with high capacity in porous and conductive flexible nanofibers represents an effective method of achieving binder-free electrode with good electrochemical performance towards wearable energy storage devices.
Aqueous zinc-ion batteries (ZIBs) have attracted significant attentions because of low cost and high reliability. However, conventional ZIBs are severely limited by the development of high energy density cathode materials with reversible Zn2+ insertion/extraction. Herein, a conducting polymer intercalated MoO3 (PMO) with extensively extended interlayer spacing is developed as a high-performance ZIBs cathode material. The interlayer spacing of PMO is prominently increased which results in an improved Zn2+ mobility during charge and discharge process. More significantly, the electrochemical results reveals that the intercalation of PANI facilitates the charge storage and reinforces the layered structure of MoO3, leading to a high capacity and good cycling stability. DFT calculation further reveals the intercalation of PANI into MoO3 significantly lower Zn2+ diffusion barrier. Benefit from these advantages, the ZIBs based on PMO electrode delivers a considerable capacity of 157 mAh/g at 0.5 A/g and ameliorative stability with 63.4% capacity retention after 1000 cycles.
Self-doping cathode interfacial layers (CILs) with both favorable electron injection and transport characteristics meet the key requirement for realizing high-performance optoelectronic devices with simplified structures. Herein, four different polypyridinium salts with tunable backbones, side chains and counter-ions are elaborately designed to afford them desirable film-forming property, polarity, structural rigidity and self-doping feature. All-solution-processed red quantum dot light-emitting diodes (QLEDs) employing them as bifunctional CILs render remarkably improved device performances in contrast to the typical CIL material of poly[(9,9-bis(30-(N,N-dimethylamino)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)] (PFN). The maximum external quantum efficiency of 2.74% achieved in this work represents one of the best values among the all-solution-processed QLEDs with individual organic CILs.
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