Latest ArticlesHybrid metal-organic framework (MOF) derivatives play a significant role in the novel catalyst development in energy conversion reactions. Here, we demonstrated the low-temperature fully fluorinated zeolitic imidazole framework (ZIF) coupled with a three-dimensional open framework Prussian blue analog (PBA) with combined advantages for electrocatalytic oxygen evolution reaction (OER) in water splitting reaction. The spectroscopic analysis and the electrochemical studies revealed the combined advantages of efficient electronic effect and active site synergism. Because of good conductivity improvement by N-doped carbon derived from ZIF and the high electrochemical surface area and active site exposure from PBA derivatives, good catalytic performance was obtained on the optimal catalyst of CoNi ZIF/CoFe-PBA-F-300, which required a low overpotential of 250 mV to reach 10 mA/cm2 loaded on the glassy carbon electrode, with Tafel slope of 47.4 mV/dec, and very high dynamic and steady stability. In addition, the multi-component with the mixed structure from highly polar metal fluorides promoted the easy formation of the active phase as revealed by the post-sample analysis. The current results showed a novel composite catalyst materials development from the hybrid MOF derivatives, which would be promising in the electrolysis of water oxidation reactions and energy-relevant catalysis reactions.
The addition of electrolyte additives is an effective strategy for tuning the property of the electrolyte to engineer the electrode/electrolyte interface, and there exist obvious discrepancies regarding the effect of fluoroethylene carbonate (FEC) as an electrolyte additive on the performance of cathodes. Herein FEC is introduced into the electrolyte of the LiMn0.8Fe0.2PO4/Li cell and its effect on the properties of the LiMn0.8Fe0.2PO4 is investigated. It is found that the addition of FEC in the electrolyte has a positive effect on the performance of the LiMn0.8Fe0.2PO4 cathode, which can be attributed to the reduced products generated by the interfacial side-reactions on the LiMn0.8Fe0.2PO4 cathode surface and the decreased metal dissolution in the FEC-containing electrolyte, thanks to the higher oxidation resistance of FEC and the easier and stronger binding of FEC and PF6−.
Molecular ferroelectrics have attracted much attention because of their excellent piezoelectricity, mechanical workability, and second harmonic effect. Here, we successfully prepared two molecular ferroelectrics 1,5–3.2.2-HdabcniX (X = ClO4−, 1; ReO4−, 2) by reactions of a quasi-spherical amine 1,5-diazabicycle[3.2.2]nonane (1.5–3.2.2-dabcn) with HX aqueous solution. Compounds 1 and 2 undergo high-temperature phase transitions at 381 K (1) and 396 K (2). Before and after the phase transition, they crystallize in the polar point group mm2, and the centrosymmetric point groups mmm and 4/mmm, respectively. According to Aizu rules, these two compounds experience mmmFmm2 and 4/mmmFmm2 type ferroelectric phase transitions, respectively. The ferroelectricity of both compounds is well expressed in their polycrystalline film at room temperature with low coercive voltages of 13 V for 1 and 25 V for 2. Using piezoelectric force microscopy (PFM), the 180° anti-parallel ferroelectric domains and the reversible polarization switching can be clearly observed in 1 and 2. This high-temperature molecular ferroelectric material has great application potential in flexible materials, biomechanics, intelligent wearables and other fields.
Lithium (Li) metal anodes (LMAs) have garnered significant attention as a potential solution for developing high-energy density batteries, given their theoretical specific capacity and redox potential. However, safety concerns and internal cycling stability issues originated from uncontrollable Li dendrite growth have impeded the practical application of LMAs. Probing the interface between Li metal and electrolyte is a crucial process that offers valuable insights into the characteristics and regularity of primary circular reactions. To illustrate the intrinsic characteristic of Li metal batteries (LMBs) in spatial and temporal, it is imperative to employ electron microscopes to characterize the structural components distribution of Li with atomic resolution. This paper summarizes the progress in the characterization and analysis of the interfaces in LMBs with electron microscopes based on the principles of electron-matter interactions. Finally, future trends and the potential of electron microscopes are also discussed to advance our understanding of LMBs.
Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal batteries. In this study, a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient Li metal anode. The polyvinyl chloride (PVC) can effectively resist water and oxygen, which is confirmed by density functional theory. The organic-dominant solid electrolyte interphases (SEI) with lithium chloride are investigated by the X-ray photoelectron spectroscopy (XPS) with little mineralization of oxide, such as Li2O and Li2CO3. With such artificial SEI, a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 mA/cm2. Moreover, the simple and convenient protected anode also exhibits excellent battery stability when paired with the LiNi0.8Co0.1Mn0.1O2 (NCM811) and LiFePO4 (LFP) cathode, showing great potential for the commercial application of lithium metal batteries.
Inspired by our previous studies to discover novel human immunodeficiency virus-1 (HIV-1) non-nucleoside reverse transcriptase inhibitors (NNRTIs) by targeting the tolerant region II of the NNRTIs binding pocket (NNIBP), a series of novel benzo[4,5]thieno[2,3-d]pyrimidine derivatives were designed through structure-based drug design as novel potent HIV-1 NNRTIs. The results showed that compound 16b was the most active inhibitor, exhibiting 50% effective concentration (EC50) values from 0.021 µmol/L to 0.298 µmol/L against wild-type (WT) and a panel of NNRTIs-resistant HIV-1 strains. Moreover, 16b was demonstrated with a significantly low 50% cytotoxicity concentration (CC50) value (> 200 µmol/L) and high selectivity index (SI) values. In addition, 16b yielded moderate reverse transcriptase (RT) enzyme inhibition with a 50% inhibition concentration (IC50) value of 0.183 µmol/L, which demonstrated that it acted as HIV-1 NNRTIs. The binding mode of 16b with RT was also illustrated via molecular docking. Overall, this work provided a novel lead compound for developing potent HIV-1 NNRTIs.
Integrating ring-fused modification with π-conjugated extension is an effective approach for designing, synthesizing, and application for novel borondipyrromethene (BODIPY) structures. In this work, based on phenyl[b]-fused BODIPY, we made reasonable modification of the methyl group at 1-site to generate dye NBDP. NBDP possessed near-infrared region (NIR) absorption and emission properties, and the intramolecular charge transfer (ICT) resulted in low fluorescence. Whereas, heat energy is evidently released in the presence of light, which can be exploited for intracellular photothermal therapy via the cell apoptosis process, reducing the inflammatory side-effects induced by necrosis. This research provides a crucial foundation for the novel molecule via BODIPY multi-directional alteration and its potential application in anti-tumor phototherapy.
The first phloroglucinol-triterpenoid hybrids, myrtphlotritins A–E (1–5), were rapidly recognized and isolated from two species of Myrtaceae by employing the building blocks-based molecular network (BBMN) strategy. Compounds 1–5 featured new carbon skeletons in which phloroglucinol derivatives were coupled with lupane- and dammarane-type triterpenoids through different linkage patterns. Their structures and absolute configurations were elucidated by comprehensive analysis of spectroscopic data and quantum chemical calculations. Biosynthetic pathways for compounds 1–5 were proposed on the basis of the coexisting precursors. Guided by the biogenetic pathways, the biomimetic synthesis of compound 1 was also achieved. Additionally, compounds 2, 3, and 5 exhibited potent antiviral activities against herpes simplex virus type-1 (HSV-1) infection, and compounds 2 and 5 displayed significant anti-inflammatory activities on RAW264.7 cells.
Surface modification of microporous bone scaffolds using nanoparticles has been broadly studied in bone tissue engineering. Aiming at improving vascularized bone regeneration (VBR), zeolitic imidazolate framework-8 (ZIF-8) was encapsulated with dimethyloxallyl glycine (DMOG) and the drug-carrying nanoparticles (D@Z) could be uniformly coated onto the surface of the bone scaffold. The osteogenic and angiogenic actions of D@Z are closely correlated with the amount of slowly released DMOG, and in general, exhibited a favorable association. Then, the D7.5@Z group, which showed the greatest capacity to induce in vitro osteogenesis–angiogenesis coupling, was utilized for surface modification of the bone scaffold. Biological processes including phosphate-containing compound metabolic process, cell differentiation, cell proliferation and cell motility might contribute to enhanced ability to induce VBR by the coated scaffold and signaling pathways such as Rap1, Ras, phosphatidylinositol 3-kinase/protein kinase B (PI3K-AKT) and vascular endothelial growth factor (VEGF) signaling pathways participated in these processes. Finally, as depicted by in vitro real time-polymerase chain reaction (RT-PCR), Western blot (WB) and in vivo cranial bone defect model, the microporous scaffold coated with nano-D7.5@Z greatly promoted VBR. To conclude, nano-D@Z has significant promise for practical application in modification of microporous bone scaffolds to enhance VBR, and DMOG loading quantity has a beneficial influence on D@Z to improve osteogenesis–angiogenesis coupling.
Abnormal accumulation and metabolism of lipid droplets can lead to a variety of diseases. Polarity, a key parameter of the microenvironment, is closely associated with many diseases and dysfunctions in the body. It is important to elucidate the relationship between the physiological activity of lipid droplets (LDs) and the polarity of the microenvironment. In this work, based on push-pull mechanism, a fluorescent probe (E)-3-(5-(4-(diphenylamino)phenyl)thiophen-2-yl)-1-(2-hydroxyphenyl)prop-2-en-1-one (PPTH) with aggregation-induced emission (AIE) properties for the detection of polarity changes in cells was synthesized. PPTH not only visualize intracellular polarity fluctuation of iron death and inflammation but also distinguish between normal and fatty liver tissue.
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