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Greer A Vassilikogiannakis G Lee KC Koffas TS Nahm K Foote CS 《The Journal of organic chemistry》2000,65(21):6876-6878
We report the effects of added acid in the reaction of singlet oxygen with trans-4-propenylanisole (1). We provide evidence that solvent acidity modifies the behavior of the transient intermediates. Relative to reactions in aprotic solvent, enhanced dioxetane concentrations are observed in MeOH and in nonprotic solvents with acid. We suggest a new mechanism that invokes a proton transfer from MeOH and benzoic acid to perepoxide (2) and zwitterion (3) intermediates. 相似文献
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Ackerman N Aharmim B Auger M Auty DJ Barbeau PS Barry K Bartoszek L Beauchamp E Belov V Benitez-Medina C Breidenbach M Burenkov A Cleveland B Conley R Conti E Cook J Cook S Coppens A Counts I Craddock W Daniels T Danilov MV Davis CG Davis J deVoe R Djurcic Z Dobi A Dolgolenko AG Dolinski MJ Donato K Dunford M Fairbank W Farine J Fierlinger P Franco D Freytag D Giroux G Gornea R Graham K Gratta G Green MP Hägemann C Hall C Hall K Haller G Hargrove C Herbst R Herrin S Hodgson J Hughes M Johnson A 《Physical review letters》2011,107(21):212501
We report the observation of two-neutrino double-beta decay in (136)Xe with T(1/2) = 2.11 ± 0.04(stat) ± 0.21(syst) × 10(21) yr. This second-order process, predicted by the standard model, has been observed for several nuclei but not for (136)Xe. The observed decay rate provides new input to matrix element calculations and to the search for the more interesting neutrinoless double-beta decay, the most sensitive probe for the existence of Majorana particles and the measurement of the neutrino mass scale. 相似文献
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Kim J Koffas TS Lawrence CC Somorjai GA 《Langmuir : the ACS journal of surfaces and colloids》2004,20(11):4640-4646
Structural investigations of bare and surface-modified polystyrene microspheres (beads) have been carried out by infrared-visible sum frequency generation (SFG) vibrational spectroscopy and scanning force microscopy (SFM). Bead surfaces have been modified by either the covalent linking of immunoglobulin G (IgG) and bovine serum albumin (BSA) or the nonspecific adsorption of a Pluronic surfactant. After surface modification with protein, SFG signals in the aliphatic CH-stretch region are detected at both the buffer/bead and air/bead interfaces, indicating that some amino acid residues in proteins adopt preferred orientations. SFG results indicate that the hydrophobic poly(propylene glycol) moieties in the Pluronic order when adsorbed onto the bead, at both the buffer/bead and air/bead interfaces, whereas hydrophilic poly(ethylene glycol) groups align to a lesser extent. SFG spectra also show that the phenyl rings of bare polystyrene beads in contact with air or buffer are ordered, with a dipole component directed along the surface normal, but become less ordered after the adsorption of either proteins or the polymer. Molecular orientation and ordering at the bead surface affect its hydrophobicity and aggregation behavior. SFM results reveal the formation of nonuniform islands when bare beads with more hydrophobic character are spun-cast onto a silica substrate. In the presence of adsorbed protein, a hexagonal packing of beads, with some defects, is observed, depending on the bulk pH and the type of attached protein. Adsorbed Pluronic causes the beads to aggregate in a disordered fashion, as compared to the behavior of bare and protein-modified beads. 相似文献
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Brady F. Cress Ujjwal Bhaskar Deepika Vaidyanathan Asher Williams Chao Cai Xinyue Liu Li Fu Vandhana M‐Chari Fuming Zhang Shaker A. Mousa Jonathan S. Dordick Mattheos A. G. Koffas Robert J. Linhardt 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(18):6023-6027
Heparin is a highly sulfated, complex polysaccharide and widely used anticoagulant pharmaceutical. In this work, we chemoenzymatically synthesized perdeuteroheparin from biosynthetically enriched heparosan precursor obtained from microbial culture in deuterated medium. Chemical de‐N‐acetylation, chemical N‐sulfation, enzymatic epimerization, and enzymatic sulfation with recombinant heparin biosynthetic enzymes afforded perdeuteroheparin comparable to pharmaceutical heparin. A series of applications for heavy heparin and its heavy biosynthetic intermediates are demonstrated, including generation of stable isotope labeled disaccharide standards, development of a non‐radioactive NMR assay for glucuronosyl‐C5‐epimerase, and background‐free quantification of in vivo half‐life following administration to rabbits. We anticipate that this approach can be extended to produce other isotope‐enriched glycosaminoglycans. 相似文献
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Nonlinear nonstationary models for time series are considered, where the series is generated from an autoregressive equation
whose coefficients change both according to time and the delayed values of the series itself, switching between several regimes.
The transition from one regime to the next one may be discontinuous (self-exciting threshold model), smooth (smooth transition
model) or continuous linear (piecewise linear threshold model). A genetic algorithm for identifying and estimating such models
is proposed, and its behavior is evaluated through a simulation study and application to temperature data and a financial
index. 相似文献
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Wenya Wang Jacob A. Englaender Peng Xu Krunal K. Mehta Jiraporn Suwan Jonathan S. Dordick Fuming Zhang Qipeng Yuan Robert J. Linhardt Mattheos Koffas 《Applied biochemistry and biotechnology》2013,171(4):954-962
A key enzyme for the biosynthesis and bioengineering of heparin, 3-O-sulfotransferase-1 (3-OST-1), was expressed and purified in Gram-positive Bacillus subtilis and Bacillus megaterium. Western blotting, protein sequence analysis, and enzyme activity measurement confirmed the expression. The enzymatic activity of 3-OST-1 expressed in Bacillus species were found to be similar to those found when expressed in Escherichia coli. The endotoxin level in 3-OST-1 from B. subtilis and B. megaterium were 104–105-fold lower than that of the E. coli-expressed 3-OST-1, which makes the Bacillus expression system of particular interest for the generation of pharmaceutical grade raw heparin from nonanimal sources. 相似文献
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Combinatorial mutasynthesis of flavonoid analogues from acrylic acids in microorganisms 总被引:5,自引:0,他引:5
Flavonoids are plant secondary metabolites often used as nutraceutical supplements, but a growing number of unnatural flavonoids are being investigated as therapeutic agents. Cultures of Saccharomyces cerevisiae expressing recombinant flavonoid enzymes, including 4-coumaroyl:CoA ligase (4CL), chalcone synthase (CHS), chalcone isomerase (CHI), and flavanone 3beta-hydroxylase (FHT), produced novel flavanones and dihydroflavonols when fed with a number of aromatic acrylic acids. The flavonoid network also exhibited broad substrate specificity by converting muconic acid into a unique polypropanoid. 相似文献
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Brady F. Cress Ujjwal Bhaskar Deepika Vaidyanathan Asher Williams Chao Cai Xinyue Liu Li Fu Vandhana M‐Chari Fuming Zhang Shaker A. Mousa Jonathan S. Dordick Mattheos A. G. Koffas Robert J. Linhardt 《Angewandte Chemie (International ed. in English)》2019,58(18):5962-5966
Heparin is a highly sulfated, complex polysaccharide and widely used anticoagulant pharmaceutical. In this work, we chemoenzymatically synthesized perdeuteroheparin from biosynthetically enriched heparosan precursor obtained from microbial culture in deuterated medium. Chemical de‐N‐acetylation, chemical N‐sulfation, enzymatic epimerization, and enzymatic sulfation with recombinant heparin biosynthetic enzymes afforded perdeuteroheparin comparable to pharmaceutical heparin. A series of applications for heavy heparin and its heavy biosynthetic intermediates are demonstrated, including generation of stable isotope labeled disaccharide standards, development of a non‐radioactive NMR assay for glucuronosyl‐C5‐epimerase, and background‐free quantification of in vivo half‐life following administration to rabbits. We anticipate that this approach can be extended to produce other isotope‐enriched glycosaminoglycans. 相似文献
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