The clinical features and immune responses of asymptomatic individuals infected with severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) have not been well described. We studied 37 ...asymptomatic individuals in the Wanzhou District who were diagnosed with RT-PCR-confirmed SARS-CoV-2 infections but without any relevant clinical symptoms in the preceding 14 d and during hospitalization. Asymptomatic individuals were admitted to the government-designated Wanzhou People's Hospital for centralized isolation in accordance with policy
. The median duration of viral shedding in the asymptomatic group was 19 d (interquartile range (IQR), 15-26 d). The asymptomatic group had a significantly longer duration of viral shedding than the symptomatic group (log-rank P = 0.028). The virus-specific IgG levels in the asymptomatic group (median S/CO, 3.4; IQR, 1.6-10.7) were significantly lower (P = 0.005) relative to the symptomatic group (median S/CO, 20.5; IQR, 5.8-38.2) in the acute phase. Of asymptomatic individuals, 93.3% (28/30) and 81.1% (30/37) had reduction in IgG and neutralizing antibody levels, respectively, during the early convalescent phase, as compared to 96.8% (30/31) and 62.2% (23/37) of symptomatic patients. Forty percent of asymptomatic individuals became seronegative and 12.9% of the symptomatic group became negative for IgG in the early convalescent phase. In addition, asymptomatic individuals exhibited lower levels of 18 pro- and anti-inflammatory cytokines. These data suggest that asymptomatic individuals had a weaker immune response to SARS-CoV-2 infection. The reduction in IgG and neutralizing antibody levels in the early convalescent phase might have implications for immunity strategy and serological surveys.
The anomalous Hall effect is a fundamental transport process in solids arising from the spin-orbit coupling. In a quantum anomalous Hall insulator, spontaneous magnetic moments and spin-orbit ...coupling combine to give rise to a topologically nontrivial electronic structure, leading to the quantized Hall effect without an external magnetic field. Based on first-principles calculations, we predict that the tetradymite semiconductors Bi₂Te₃, Bi₂Se₃, and Sb₂Te₃ form magnetically ordered insulators when doped with transition metal elements (Cr or Fe), in contrast to conventional dilute magnetic semiconductors where free carriers are necessary to mediate the magnetic coupling. In two-dimensional thin films, this magnetic order gives rise to a topological electronic structure characterized by a finite Chern number, with the Hall conductance quantized in units of e²/h (where e is the charge of an electron and h is Planck's constant).
Background Large area skin trauma has always been a great challenge for both patients and clinicians. Exosomes originating from human adipose-derived mesenchymal stem cells (hADSCs) have been a novel ...promising cell-free treatment in cutaneous damage repair. Nevertheless, the low retention rate of exosomes post-transplantation in vivo remains a significant challenge in clinical applications. Herein, we purposed to explore the potential clinical application roles of hADSCs-Exos encapsulated in functional PF-127 hydrogel in wound healing. Methods hADSCs-Exos were isolated from human hADSCs by ultracentrifugation. An injectable, biocompatible, and thermo-sensitive hydrogel Pluronic F-127 hydrogel was employed to encapsulate allogeneic hADSCs-Exos, and this complex was topically applied to a full-thickness cutaneous wound in mice. On different days post-transplantation, the mice were sacrificed, and the skin tissue was excised for histological and immunohistochemical analysis. Results Compared with hADSCs-Exos or PF-127 only, PF-127/hADSCs-Exos complexes enhanced skin wound healing, promoted re-epithelialization, increased expression of Ki67, alpha-SMA, and CD31, facilitated collagen synthesis (Collagen I, Collagen III), up-regulated expression of skin barrier proteins (KRT1, AQP3), and reduced inflammation (IL-6, TNF-alpha, CD68, CD206). By using PF-127/hADSCs-Exos complexes, hADSCs-Exos can be administrated at lower doses frequency while maintaining the same therapeutic effects. Conclusion Administration of hADSCs-Exos in PF-127 improves the efficiency of exosome delivery, maintains the bioactivity of hADSCs-Exos, and optimizes the performance of hADSCs-Exos. Thus, this biomaterial-based exosome will be a promising treatment approach for the cutaneous rejuvenation of skin wounds. Keywords: Wound healing, Adipose-derived mesenchymal stem cells, Exosomes, PF-127 hydrogel
Fluorinated ketones are widely prevalent in numerous biologically interesting molecules, and the development of novel transformations to access these structures is an important task in organic ...synthesis. Herein, we report the multicomponent radical acylfluoroalkylation of a variety of olefins in the presence of various commercially available aromatic aldehydes and fluoroalkyl reagents through N‐heterocyclic carbene organocatalysis. With this protocol, over 120 examples of functionalized ketones with diverse fluorine substituents have been synthesized in up to 99 % yield with complete regioselectivity. The generality of this catalytic strategy was further highlighted by its successful application in the late‐stage functionalization of pharmaceutical skeletons. Excellent diastereoselectivity could be achieved in the reactions forging multiple stereocenters. In addition, preliminary results have been achieved on the catalytic asymmetric variant of the olefin difunctionalization process.
Organocatalytic acylfluoroalkylation: A multicomponent radical acylfluoroalkylation of olefins through NHC organocatalysis was developed, and over 120 examples of fluoroketones were facilely accessed from simple materials. Moreover, a dearomative difunctionalization of indoles could be readily achieved in a highly diastereoselective manner. The generality and practicality were highlighted by the late‐stage modification of drug skeletons.
Highly efficient hydrogen evolution reaction (HER) electrocatalyst will determine the mass distributions of hydrogen‐powered clean technologies, while still faces grand challenges. In this work, a ...synergistic ligand modulation plus Co doping strategy is applied to 1T−MoS2 catalyst via CoMo‐metal‐organic frameworks precursors, boosting the HER catalytic activity and durability of 1T−MoS2. Confirmed by Cs corrected transmission electron microscope and X‐ray absorption spectroscopy, the polydentate 1,2‐bis(4‐pyridyl)ethane ligand can stably link with two‐dimensional 1T−MoS2 layers through cobalt sites to expand interlayer spacing of MoS2 (Co−1T−MoS2‐bpe), which promotes active site exposure, accelerates water dissociation, and optimizes the adsorption and desorption of H in alkaline HER processes. Theoretical calculations indicate the promotions in the electronic structure of 1T−MoS2 originate in the formation of three‐dimensional metal‐organic constructs by linking π‐conjugated ligand, which weakens the hybridization between Mo‐3d and S‐2p orbitals, and in turn makes S‐2p orbital more suitable for hybridization with H‐1s orbital. Therefore, Co−1T−MoS2‐bpe exhibits excellent stability and exceedingly low overpotential for alkaline HER (118 mV at 10 mA cm−2). In addition, integrated into an anion‐exchange membrane water electrolyzer, Co−1T−MoS2‐bpe is much superior to the Pt/C catalyst at the large current densities. This study provides a feasible ligand modulation strategy for designs of two‐dimensional catalysts.
A synergistic ligand modulation plus cobalt doping strategy is applied to modulate the orbital hybridization of 1T‐MoS2 catalyst via CoMo‐MOF precursors. The polydentate 1,2‐bis(4‐pyridyl)ethane (bpe) ligand can stably link with 1T‐MoS2 layers to achieve expanded interlayer spacing, which promotes the joint participation of highly efficient active sites in the basal plane and the interlayer in alkaline HER processes.
Asymmetric Total Synthesis of (+)‐Mannolide C Ao, Qiaoqiao; Zhang, Hai‐Jun; Zheng, Jinbin ...
Angewandte Chemie International Edition,
September 20, 2021, Letnik:
60, Številka:
39
Journal Article
Recenzirano
(+)‐Mannolide C is a complex hexacyclic C20 cephalotane‐type diterpenoid featuring a highly strained 7/6/6/5 tetracyclic core containing eight consecutive stereocenters and two bridging lactones. The ...first asymmetric total synthesis of (+)‐mannolide C has been accomplished by lipase‐mediated resolution, Ru‐complex‐catalyzed double ring‐closing metathesis (RCM) reactions, NiII‐catalyzed diastereoselective Michael addition, and MnIII‐catalyzed allylic oxidation as the key transformations.
The first asymmetric total synthesis of (+)‐mannolide C, a highly strained bowl‐shaped cephalotane‐type diterpenoid is reported. The synthetic strategy features efficient double ring‐closing metathesis reactions for the formation of the highly strained bowl‐shaped 7/6/6/5 tetracyclic system.
A strategically novel synthetic method for the fluoroarylation of allenic ester was developed that enables the expedient construction of a host of β‐fluoroalkyl‐containing cinnamate derivatives. The ...reaction proceeds through visible‐light‐promoted gold redox catalysis, occurs smoothly under very mild reaction conditions, accommodates a large variety of functional groups, and more importantly allows the incorporation of fluorine and aryl groups with excellent regio‐ and stereoselectivity. The concomitant activation mode for both the allene motif and the hydrogen fluoride is key for the success of the reaction.
Leading light: A regio‐ and stereoselective fluoroarylation of allenic esters through visible‐light‐promoted gold redox catalysis with cost‐effective Et3N⋅3 HF as the nucleophilic fluorine source is reported. Preliminary mechanistic studies reveal concomitant activation of the allene motif by a high‐valent gold complex and the hydrogen fluoride by hydrogen bonding with the ester group, thereby enabling the otherwise challenging fluorine incorporation.
The formation of aryl‐alkyl ether bonds through cross coupling of alcohols with aryl halides represents a useful strategic departure from classical SN2 methods. Numerous tactics relying on Pd‐, Cu‐, ...and Ni‐based catalytic systems have emerged over the past several years. Herein we disclose a Ni‐catalyzed electrochemically driven protocol to achieve this useful transformation with a broad substrate scope in an operationally simple way. This electrochemical method does not require strong base, exogenous expensive transition metal catalysts (e.g., Ir, Ru), and can easily be scaled up in either a batch or flow setting. Interestingly, e‐etherification exhibits an enhanced substrate scope over the mechanistically related photochemical variant as it tolerates tertiary amine functional groups in the alcohol nucleophile.
Highly chemoselective O‐arylation was achieved by electrochemically‐driven nickel catalysis. This method exhibits broad substrate scope comparable to state‐of‐the‐art Pd, Cu and photochemically facilitated Ni catalysis. This e‐etherification forged ether bonds in demanding settings where other methods failed. With its excellent scalability, this work represents a modular, mild, and simple ether bond formation for contemporary medicinal chemistry.
Conversion of levulinic acid to valuable chemicals: a review Xu, Wen‐Ping; Chen, Xue‐Fang; Guo, Hai‐Jun ...
Journal of chemical technology and biotechnology (1986),
November 2021, 2021-11-00, 20211101, Letnik:
96, Številka:
11
Journal Article
Decycling and dismantling of complex networks are underlying many important applications in network science. Recently these two closely related problems were tackled by several heuristic algorithms, ...simple and considerably sub-optimal, on the one hand, and involved and accurate message-passing ones that evaluate single-node marginal probabilities, on the other hand. In this paper we propose a simple and extremely fast algorithm, CoreHD, which recursively removes nodes of the highest degree from the 2-core of the network. CoreHD performs much better than all existing simple algorithms. When applied on real-world networks, it achieves equally good solutions as those obtained by the state-of-art iterative message-passing algorithms at greatly reduced computational cost, suggesting that CoreHD should be the algorithm of choice for many practical purposes.
PDF
