Latest ArticlesAssembling MnO2 nanowires into macroscopic membrane is a promising engineered technology for catalyst separation and enhancement of Fenton-like reaction activity, yet its development is limited by the deficiencies in preparation and property modulation of the MnO2 nanowires. In this work, we developed a facile method using C2H5OH and CH3COOK as reductive and vital control reagents to react with KMnO4 by hydrothermal reaction at 140 ℃ for 12 h, to prepare the ultralong α-MnO2 nanowires up to tens of micrometers with high purity and aspect ratio. Such strategy not only had the advantages of being mild, easily controlled and environmental pollution-free, but also endowed α-MnO2 nanowires with excellent ability as a Fenton catalyst when assembled into free-standing membrane for degrading phenolic compounds (kobs = 0.0738 ~ 0.1695 min−1) in a continuous flow reaction. The reactive oxygen species (i.e., •OH) from Fenton-like reaction were enriched within this α-MnO2 nanowire membrane via nanoconfinement effect, which further enhanced the mass transportation of •OH available for phenolic contaminants. MnO2 nanowire membrane using our method possessed the high practical potential for water purify due to its easy-preparation and enhanced catalytic performances.
Palladium-catalyzed non-directed CH functionalization provides an efficient approach for direct functionalization of arenes, but it usually suffers from poor site selectivity, limiting its wide application. Herein, it is reported for the first time that the carboxylic acid ligand of 3, 5-dimethyladamantane-1-carboxylic acid (1-DMAdCO2H) can affect the site selectivity during the CH activation step in palladium-catalyzed non-directed CH functionalization, leading to highly para-selective CH olefination of TIPS-protected phenols. This transformation displayed good generality in realizing various other para-selective CH functionalization reactions such as halogenation, and allylation reactions. A wide variety of phenol derivatives including bioactive molecules of triclosan, thymol, and propofol, were compatible substrates, leading to the corresponding para-selective products in moderate to good yields. A preliminary mechanism study revealed that the spatial repulsion factor between carboxylic acid ligand and bulky protecting group resulted in the selective CH activation at the less sterically hindered para-position. This new model non-directed para-selective CH functionalization can provide a straightforward route for remote site-selective CH activations.
A cobalt-catalyzed ring-opening/hydroxylation cascade of highly strained cyclopropanols has been developed for the first time. The reaction was conducted under open-air atmosphere to afford a broad series of structurally diverse β-hydroxy ketones in moderate to good yields with high regioselectivity. The protocol features mild reaction conditions, simple operation, high-functional-group tolerance, facile scalability, and heterocycle compatibility.
HIV-1 capsid protein (CA) has emerged as a promising target for antiviral treatment considering its structural and regulatory roles in HIV-1 replication. Here, we disclose the design, synthesis, biological assessment, and mechanism investigation of a novel series of phenylalanine derivatives gained by further structural modification of PF74. The newly synthesized compounds demonstrated potent anti-HIV activity, represented by 7n displayed anti-HIV-1 activity 6.25-fold better than PF74, and 7h showed anti-HIV-2 activity with nearly 139 times improved efficacy over PF74. Surface plasmon resonance (SPR) studies of representative compounds proved that HIV-1 CA was the binding target. Competitive SPR studies using CPSF6 and NUP153 peptides identified that 7n binds to a vital CA assembly interface between the N-terminal and C-terminal domain (NTD-CTD interface). Action stage determination assay revealed that the newly synthesized compounds were antiviral with a dual-stage inhibitory profile. Molecular dynamics (MD) simulations offered the crucial foundation for the hopeful antiviral potency of 7n. Besides, 7m and 7n modestly increased metabolic stabilities in human liver microsome (HLM) and human plasma compared to PF74. Overall, these studies offer valuable insights and can regard as the beginning for succedent medicinal chemistry endeavors to discover promising HIV capsid inhibitors with improved efficacy and better drug-like characteristics.
It is of great significance to construct organic circularly polarized luminescence systems (CPL) with large luminescence dissymmetry factors (glum) for practical applications. Here we report organic CPL systems constructed by merging triplet-triplet annihilation upconversion chromophores in cellulose matrices. The chirality of the matrix is transferred to the achiral chromophores of photon upconversion and then the multistep energy transfer processes of upconversion amplify glum. The glum value of upconversion CPL in the left-handed ethyl cellulose and the right-handed (acetyl) ethyl cellulose are up to +0.1 and −0.15, respectively. The study provides a straightforward approach for constructing solid organic upconversion CPL materials with large glum, which may expand the application potentials of organic chiroptical materials.
Alkaline phosphatase (ALP) activity assay is not only significant to the clinical diagnosis of some related disease, but also momentous to the construction of ALP-based enzyme-linked immunosorbent assay (ELISA). Herein, for the first time, we have discovered that ascorbic acid (AA) can specially react with N-methylethylenediamine (N-MEDA) to generate fluorescent non-conjugated polymer dots (NCPDs) under mild conditions. On the basis of the AA-responsive emission and ALP-catalyzed hydrolysis of ascorbic acid 2-phosphate (AA2P) to AA, we have exploited a fluorometric ALP activity assay with high sensitivity and selectivity. Furthermore, by means of conventional ALP-based ELISA platform, a conceptual fluorescent ELISA has been constructed and applied in the potential clinical diagnosis, during which cardiac troponin I (cTnI), a well-established biomarker of acute myocardial infarction, has been chosen as the model target. We envision that such original fluorescent NCPDs generation-enabled ELISA could become a versatile tool in biochemical sensing and medical diagnosis in the future.
Liposomes have been widely exploited as a drug delivery system in treating tumors because of their advantage to enhance anti-tumor efficacy and reduce side effects. In this study, the tumor-targeted 2-dodecyl-6-methoxycyclohexa-2, 5-diene-1, 4-dione (DMDD, i.e., Averrhoa carambola extractive) liposomes (HA/TN-DLP) were conducted and assessed. HA/TN-DLP showed controllable drug loading (up to 83%) with high stability. In vitro and in vivo studies showed good cell uptake behavior and high inhibition rate of breast cancer compared to free DMDD. HA/TN-DLP might be the suitable for DMDD due to its better advantages in delivery, penetrability, and targeting-tumor capability. For in vivo mouse model tests, HA/TN-DLP effectively inhibited tumor growth compared to free DMDD. Further analyses indicated that HA/TN-DLP inhibited the glycerophospholipid metabolism pathway by reducing the biosynthesis of phosphatidylcholine and 1-acyl-sn-glycero-3-phosphocholine through regulating the expressions of CEPT1 and LYPLA1, and inhibited tumor cell growth by regulating the PI3K/Akt and NF-κB signaling pathways. In conclusion, the obviously enhanced antitumor effect further demonstrated that HA/TN-DLP may be a promising tumor-targeting agent.
We demonstrate a synaptic transistor that uses a thermally crosslinked three-dimensional network to accommodate ionic liquid to form an ion gel layer. The synaptic transistor successfully emulated important synaptic plasticity, such as paired-pulse facilitation, spike-number dependent plasticity, spike-voltage dependent plasticity, and spike-rate dependent plasticity; these responses imply successful use of the ion gel. Moreover, the device realized "OR" and "AND" logic operations, and high-pass filtering behavior. Energy consumption of the device can be reduced to sub-femtojoule level, which is below that of biological synapses. Compared with traditional physical cross-linking using block copolymers, this method provides a facile strategy to prepare ion gels with tunable properties by altering the polymers and crosslinkers, and to enormously reduce the price by replacing expensive block copolymers or eliminating additional synthesis processes. This report provides a versatile strategy for design of synaptic transistors and their applications in neuromorphic electronics.
Sepsis is the leading cause of death in intensive care unit (ICU), which is caused by deregulated immune responses to pathogens infection. Clinically, sepsis treatment is limited to antibiotics and supportive care, while there still lacks of specific molecular therapy. As a type of immune dysfunction disease, macrophages have been recognized as the key immune cells precipitating in the whole process of sepsis, which is activated into M1-like to trigger various inflammatory responses at early stage whereas polarized into M2-like to cause immunosuppression in later stage. Therefore, great attention has been paid on the design of nanomedicines to regulate the functions of macrophages for etiological treatment of sepsis, by virtue of the unique advantages of nano-drug delivery systems, such as enhanced drug bioavailability, targetability, reduced side-effects. This critical review aims to summarize the recent progress of macrophages-regulating nanoparticles for sepsis therapy. First, the essential roles of macrophages in the development and progression of sepsis have been introduced, including the positive roles of macrophages to combat infections and dysfunction of macrophages to cause body damages. We then focus our main attention to discuss the nanomedicines with different therapeutic mechanisms corresponding to each stage of sepsis, such as infection blockage, inflammation inhibition, immune functions recovery, as well as multifunctional nanomedicines. Finally, a few limitations of current nanomedicines are highlighted, and future perspective are speculated for potential clinical translation, which might pave the way for the development of macrophages-centered nanomedicines for more effective sepsis therapy.
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