Latest ArticlesTriphenylamine (TPA) derivatives have been widely used as useful building blocks for diverse functional materials because of their excellent redox activity. Most of the molecular structures of TPA-based organic functional materials contain 4-anisyl groups, which on one hand could reduce their oxidation potential and on the other hand significantly delocalize the spin density of the resultant TPA radical cation species and enhance their stability. However, molecular-level investigation of the redox behavior of triphenylamines consisting of 4-anisyl group and the electronic structures of their radical cation species has not been reported in the literature. Herein, we design a series of triphenylamines consisting of one, two, or three 3, 5-di-tert-butyl-4-anisyl groups and investigate their redox behaviors and corresponding radical cation species. We disclose that the resonance hybrid and steric protection could both contribute to the stability of triphenylamine radical cations. Moreover, further oxidation leads to an unexpected oxidative demethylation. The findings in this work may reveal new insights for the understanding of the unique redox properties of 4-anisyl substituted triphenylamines.
Theranostic visualization of dextran at the nanoscale is beneficial for understanding the bioregulatory mechanisms of this molecule. In this study, we applied structured illumination microscopy (SIM) to capture the distribution of Cy5-Dextran at different incubation periods in living cells. The results showed that Cy5-Dextran could be absorbed by HeLa cells. In addition, we clarified that Cy5-Dextran exhibited differential organelle distribution (lysosomal or mitochondrial) in a time-dependent manner. Moreover, lysosomal Cy5-Dextran localization was found to be independent of the autophagy process, while Cy5-Dextran localized to the mitochondria triggered a pro-apoptotic event, upregulating the levels of reactive oxygen species (ROS) to accelerate mitochondrial fragmentation. This work uses a visualized strategy to reveal the anti-tumor bioactivity of dextran, which was achieved by regulating apoptosis and autophagy.
Neuroinflammation plays a significant role in inducing depression-like behavior. Tetrahedral DNA nanostructures (TDNs) are molecules that exhibit anti-inflammatory properties and can effectively penetrate the blood-brain barrier. Thus, researchers have hypothesized that TDNs regulate the secretion of proinflammatory cytokines and consequently alleviate depression-like behavior. To test this hypothesis, we investigated the effect of TDNs on the depression-like behavior of C57 mice induced by lipopolysaccharide (LPS). We performed open-field, tail suspension, and sucrose preference tests on LPS- and LPS/TDN-treated mice. The results indicated that the injection of TDNs into LPS-treated mice resulted in increased velocity, center zone duration, frequency to the center zone, and sucrose preference, and decreased immobility time. Immunofluorescence results indicated that peripheral administration of LPS in the mice activated inflammation, which culminated in distinct depression-like behavior. However, TDNs effectively alleviated the inflammation and depression-like behavior through the reduction of the expression levels of proinflammatory cytokines, such as interleukin-1β and tumor necrosis factor-α in the brain. Additionally, TDNs normalized the expression level of microglia cell activation markers, such as ionized calcium binding adaptor molecule 1, in the hippocampus of mice. These results indicated that TDNs attenuated the LPS-induced secretion of inflammatory factors and consequently alleviated depression-like behavior.
Noble metal aerogels (NMAs), belonging to the porous material, have exhibited excellent catalytic performance. Although the synthesis method continues to improve, it still exists some problems which hindered the experimental process, such as high concentration of noble metal precursors, long synthesis cycle, expensive production cost, and uncontrollable ligament length. In this work, ultrasonic wave and reducing agent NaBH4 were simultaneously applied to gelation process. With the cavitation of ultrasound, it can generate huge energy with heating and stirring, thus gelation reaction proceeded quickly, and even completed the process in only a few seconds, that is much faster than the recorded. A wide concentration range was successfully expanded from 0.02 mmol/L to 62.5 mmol/L. Further, we extended this method to a variety of noble metal elements (Au, Ru, Rh, Ag, Pt, Pd), and this method is adaptive for the synthesis of single metal aerogels (Au, Ag, Ru, Rh, Pd), bimetal and trimetal aerogels (Au-Ag, Au-Rh, Au-Ru, Au-Pt, Au-Pd, Au-Pt-Pd). In addition, the ligament size of alloy aerogels are 10 nm or less. Moreover, their brilliant properties were demonstrated in hydrogen evolution reaction (HER) and ethanol oxidation reaction (EOR).
miRNA, which is a common non-coding RNA, can target various mRNAs to regulate their physiological activities. Therefore, miRNAs play an important role in various physiological and pathological processes, and so they have been proposed as a powerful tool to treat different diseases efficiently. However, the characteristic of miRNA degradation in vivo limits its further clinical application. Exosomes have the advantage of crossing the biological barrier and achieving long-distance communication with cells, so they are excellent vectors for miRNAs. By studying the biogenesis of exosomes, the way for loading miRNAs, the mechanism of targeting, and disease occurrence and development, it is confirmed that exosomes can enrich specific endogenous miRNAs and regulate a variety of physiological activities, such as promoting cancer cell apoptosis, regulating lipid metabolism and promoting angiogenesis. It is shown that exosomes loaded with miRNAs have good performance in the fields of cancer, neurodegenerative diseases, cardiovascular disease treatment, and regenerative medicine. In this paper, the application and research progress of exosomes carrying miRNA in the above fields are systematically described.
In order to fully replace the traditional fossil energy supply system, the efficiency of electrochemical energy conversion and storage of new energy technology needs to be continuously improved to enhance its market competitiveness. The structural design of energy devices can achieve satisfactory energy conversion and storage performance. To achieve lightweight design, improve mechanical support, enhance electrochemical performance, and adapt to the special shape of the device, the structural energy devices develop very quickly. To help researchers analyze the development and get clear on developing trend, this review is prepared. This review summarizes the latest developments in structural energy devices, including special attention to fuel cells, lithium-ion batteries, lithium metal batteries, and supercapacitors. Finally, the existing problems of structural energy devices are discussed, and the current challenges and future opportunities are summarized and prospected. Structural energy devices can undoubtedly overcome the performance bottlenecks of traditional energy devices, break the limitations of existing materials and structures, and provide a guidance for the development of equipment with high performance, light weight and low cost in the future.
Artificial membrane transporters that either use chalcogen bonds to facilitate transmembrane flux of anions or show high selectivity toward perchlorate anions are rare. In this work, we report on one such novel monopeptide-based transporter system, featuring both chalcogen bonds for highly efficient anion transport and high transport selectivity toward ClO4- anions. Structurally, these monopeptide molecules associate with each other via H-bonds to produce H-bonded 1D stack that not only one dimensionally but also directionally aligns the terminal bicyclic thiophene motifs to the same side. Functionally, these well-aligned thiophenes create a sulfur-rich transmembrane pathway, combinatorially fine-tunable to enable anions to efficiently cross the membrane in the increasing activity of Cl- < Br- < NO3- < ClO4- via chalcogen bonds, with EC50 values of 0.75, 0.40, 0.37 and 0.093 μmol/L (0.3 mol% relative to lipid molecules), respectively.
Dimeric sesquiterpenoids possessing densely substituted 7-norbornenone/7-norbornenol motifs pose a considerable challenge for chemical synthesis. From a strategic perspective, one could envision intermolecular Diels−Alder cycloaddition as a straightforward method for assembling alkyl-substituted 7-norbornenones. However, this approach is hindered by lability of the required dienes, namely alkyl-substituted cyclopentadienones. Here we report a one-pot protocol for construction of alkyl-substituted 7-norbornenones from electron-deficient olefins and a cyclopentenone derivative. DDQ was found to be an effective oxidant for generating a cyclopentadienone intermediate in situ from the enone. A series of sterically congested 7-norbornenone-containing polycyclic compounds were prepared by using this protocol.
A catalytic asymmetric total synthesis of (+)-vincamine is presented. Key features of the synthesis include a Pd-catalyzed enantioselective decarboxylative allylation to form the C20 quaternary stereogenic center and a stereoselective iminium reduction to install the critical cis-C20/C21 relative stereochemisty.
The development of innovative strategies and methods to provide natural product-like macrocycles not accessible by biosynthesis, but endowed with novel bioactivities and simplified structure, is highly desirable. Inspired by the key scaffolds of rapamycin and FR252921, herein, we report a Rh(Ⅲ)-catalyzed C-H alkylation macrocyclization, which enables access to CF3-substituted macrolides. DFT calculations reveal that the chemoselectivity between C-H alkylation and olefination macrocyclization was highly controllable. Moreover, the unique CF3-substituted macrolides showed potent anti-inflammation activities against TNF-α, IL-6 and CCL2 mRNA expression.
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