Multiresponsive polyelectrolyte hydrogels with extraordinary toughness have great potential in soft device applications. Previously we have demonstrated a series of tough and multiresponsive ...hydrogels by using multifunctional triblock copolymer (Pluronic F127 diacrylate, F127DA) micelles to cross-link cationic polyelectrolyte chains into 3D network. Herein, we further synthesize negatively charged hydrogels comprising 2-acrylamido-2-methyl propylsulfonic acid (AMPS) monomers by using F127DA micelles as cross-linkers. Similar to the positive nanomicelle (NM) hydrogels, the negative NM hydrogels exhibited a compressive strength up to 59 MPa with a fracture strain up to 98%, and tensile fracture strain higher than 2000%. These charged hydrogels were actuated by electric field when immersed in salt solutions. The effects of electrolyte concentration, electric field strength, and ionic monomer content on the electric actuation behavior of these electroactive hydrogels (EAHs) have been systematically investigated. It is concluded that the electroactive hydrogels show a fast actuation rate with a bending angle up to 87° at 120 s and the bending angle was cyclically reversed upon changing bias direction without a large decrease. This study demonstrates that such tough and multiresponsive electroactive hydrogels may have great potential in sensors, actuators, switches, and artificial muscles.
Organophosphorus compounds have all along attracted considerable attention as they have broad utilities such as reagents for chemical reactions, ligands for transition metal catalysts, flame ...retardants, biologically active molecules and building blocks in synthetic chemistry. Compared with metal-catalyzed coupling synthesis, transformations via P-center radicals processes are powerful methods for the synthesis of organophosphorus compounds, as they provide unique routes leading to target molecules in least and concise steps. Generally, homolytic cleavage of P-H bonds serves as a major approach for the generation of P-centered radicals. And the reaction varieties between P-centered radicals and unsaturated compounds including addition reactions, addition/dehydrogenation reactions and difunctionalizations.
This review will focus on the difunctionalization reactions between unsaturated compounds and P-centered radicals origin from P-H compounds published in the period from 2010 to October 2016, by highlighting the reactions' specificity and, where possible, the relevant mechanistic rationale.
3-Phosphinoylindole derivatives play important roles as pharmaceutical drugs and ligands. A new method for the synthesis of 3-phosphinoylindole derivatives has been achieved through silver-mediated ...cycloaddition between N-Ts-2-alkynylaniline derivatives and H-phosphine oxides. This transformation offers a straightforward route to the formation of the C–P bond, indole ring, and desulfonylation in one step.
The first multicomponent reaction (MCR) involving aryl boronic acids, elemental sulfur, and P(O)H compounds is presented. It proceeds with excellent yields and provides an attractive approach for ...the construction of valuable S-aryl phosphorothioates and S-aryl phosphorodithioates using a one-step strategy. Moreover, this method can be easily adapted to large-scale preparation.
Emerging evidence indicates an association between gut microbiome and arthritis diseases including gout. However, how and which gut bacteria affect host urate degradation and inflammation in gout ...remains unclear. Here we performed a metagenome analysis on 307 fecal samples from 102 gout patients and 86 healthy controls. Gout metagenomes significantly differed from those of healthy controls. The relative abundances of Prevotella, Fusobacterium, and Bacteroides were increased in gout, whereas those of Enterobacteriaceae and butyrate-producing species were decreased. Functionally, gout patients had greater abundances for genes in fructose, mannose metabolism and lipid A biosynthesis, and lower for genes in urate degradation and short chain fatty acid production. A three-pronged association between metagenomic species, functions and clinical parameters revealed that decreased abundances of species in Enterobacteriaceae were associated with reduced amino acid metabolism and environmental sensing, which together contribute to increased serum uric acid and C-reactive protein levels in gout. A random forest classifier based on three gut microbial genes showed high predictivity for gout in both discovery and validation cohorts (0.91 and 0.80 accuracy), with high specificity in the context of other chronic disorders. Longitudinal analysis showed that uric-acid-lowering and anti-inflammatory drugs partially restored gut microbiota after 24-week treatment. Comparative analysis with obesity, type 2 diabetes, ankylosing spondylitis and rheumatoid arthritis indicated that gout metagenomes were more similar to those of autoimmune than metabolic diseases. Our results suggest that gut dysbiosis was associated with dysregulated host urate degradation and systemic inflammation and may be used as non-invasive diagnostic markers for gout.
The general method for the oxidative cyclization of arylacrylamides with dichloromethane or acetonitrile has been developed. The reactions described provide novel access to chloro- and ...cyano-containing oxindoles in good to moderate yields that allow the direct formation of a C-C bond and the construction of an oxindole ring in one reaction. The use of a cheap and easily prepared Mn(OAc)3 represents an added advantage of this method.
Isobaric chemical labeling is a widely used strategy for high-throughput quantitative proteomics based on mass spectrometry. However, commercially available reagents have high costs in applications ...as well as the sensitivity limitations for detection of the trace protein samples. Previously, we developed a 2-plex isobaric labeling strategy based on phosphorus chemistry for ultrasensitive proteome quantification with high accuracy. In this work, 6-plex tandem phosphorus tags (TPT) were developed with 3-fold increase in the multiplexing quantitative capacity compared to the 2-plex isobaric phosphorus reagents introduced previously. High isotope enrichment of 18O labeling was incorporated into the phosphoryl group with three exchangeable oxygen atoms by using commercially available H218O. The combinational incorporations of 18O atom in reporter ions and balance group set up the low-cost foundation for development of multiplex TPT reagents. The novel 6-plex TPT reagents could produce phosphoramidate as unique reporter ions with approximately 1 Da mass difference and thus enable 6-plex quantitative analysis in high-resolution ESI-MS/MS analysis. Using HeLa cell tryptic peptides, we concluded that 6-plex TPT reagents could facilitate large-scale accurate quantitative proteomics with very high labeling efficiency.Isobaric chemical labeling is a widely used strategy for high-throughput quantitative proteomics based on mass spectrometry. However, commercially available reagents have high costs in applications as well as the sensitivity limitations for detection of the trace protein samples. Previously, we developed a 2-plex isobaric labeling strategy based on phosphorus chemistry for ultrasensitive proteome quantification with high accuracy. In this work, 6-plex tandem phosphorus tags (TPT) were developed with 3-fold increase in the multiplexing quantitative capacity compared to the 2-plex isobaric phosphorus reagents introduced previously. High isotope enrichment of 18O labeling was incorporated into the phosphoryl group with three exchangeable oxygen atoms by using commercially available H218O. The combinational incorporations of 18O atom in reporter ions and balance group set up the low-cost foundation for development of multiplex TPT reagents. The novel 6-plex TPT reagents could produce phosphoramidate as unique reporter ions with approximately 1 Da mass difference and thus enable 6-plex quantitative analysis in high-resolution ESI-MS/MS analysis. Using HeLa cell tryptic peptides, we concluded that 6-plex TPT reagents could facilitate large-scale accurate quantitative proteomics with very high labeling efficiency.
Human blood cells (HBCs) play essential roles in multiple biological processes but their roles in development of uterine polyps are unknown. Here we implemented a Mendelian randomization (MR) ...analysis to investigate the effects of 36 HBC traits on endometrial polyps (EPs) and cervical polyps (CPs). The random-effect inverse-variance weighted method was adopted as standard MR analysis and three additional MR methods (MR-Egger, weighted median, and MR-PRESSO) were used for sensitivity analyses. Genetic instruments of HBC traits was extracted from a large genome-wide association study of 173,480 individuals, while data for EPs and CPs were obtained from the UK Biobank. All samples were Europeans. Using genetic variants as instrumental variables, our study found that both eosinophil count (OR 0.85, 95% CI 0.79-0.93, P = 1.06 × 10
) and eosinophil percentage of white cells (OR 0.84, 95% CI 0.77-0.91, P = 2.43 × 10
) were associated with decreased risk of EPs. The results were robust in sensitivity analyses and no evidences of horizontal pleiotropy were observed. While we found no significant associations between HBC traits and CPs. Our findings suggested eosinophils might play important roles in the pathogenesis of EPs. Besides, out study provided novel insight into detecting uterine polyps biomarkers using genetic epidemiology approaches.
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