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21.
22.
pH‐controlled reaction divergence of decarboxylation versus fragmentation in reactions of dihydroxyfumarate with glyoxylate and formaldehyde: parallels to biological pathways 下载免费PDF全文
Christopher J. Butch Jing Wang Jiande Gu Rebeca Vindas Jacob Crowe Pamela Pollet Leslie Gelbaum Jerzy Leszczynski Ramanarayanan Krishnamurthy Charles L. Liotta 《Journal of Physical Organic Chemistry》2016,29(7):352-360
The reactions of dihydroxyfumarate with glyoxylate and formaldehyde exhibit a unique pH‐controlled mechanistic divergence leading to different product suites by two distinct pathways. The divergent reactions proceed via a central intermediate (2,3‐dihydroxy‐oxalosuccinate, 3 , in the reaction with glyoxylate and 2‐hydroxy‐2‐hydroxymethyl‐3‐oxosuccinate, 14 , in the reaction with formaldehyde). At pH 7–8, products ( 7 , 8 , and 15 ) exclusively from a decarboxylation of the intermediate are observed, while at pH 13–14, products ( 9 , 10 , and 16 ) solely derived from a hydroxide‐promoted fragmentation of the intermediate are formed. The decarboxylative and fragmentation pathways are mutually exclusive and do not appear to coexist under the range of pH (7–14) conditions investigated. Herein, we employ a combination of quantitative 13C NMR measurements and density functional theory calculations to provide a rationale for this pH‐driven reaction divergence. These rationalizations also hold true for the reactions of dihydroxyfumarate produced in situ by the catalytic cyanide‐mediated dimerization of glyoxylate. In addition, the non‐enzymatic decarboxylation and fragmentation transformations of these central intermediates ( 3 and 14 ) appear to have intriguing parallels to the enzymatic reactions of oxalosuccinate and formation of glyceric acid derivatives in extant metabolism – the high and low pH mimicking the precise control exerted by the enzymes over reaction pathways. Copyright © 2016 John Wiley & Sons, Ltd. 相似文献
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Li T Garg U Liu Y Marks R Nayak BK Rao PV Fujiwara M Hashimoto H Kawase K Nakanishi K Okumura S Yosoi M Itoh M Ichikawa M Matsuo R Terazono T Uchida M Kawabata T Akimune H Iwao Y Murakami T Sakaguchi H Terashima S Yasuda Y Zenihiro J Harakeh MN 《Physical review letters》2007,99(16):162503
The strength distributions of the giant monopole resonance (GMR) have been measured in the even-A Sn isotopes (A=112-124) with inelastic scattering of 400-MeV alpha particles in the angular range 0 degrees -8.5 degrees . We find that the experimentally observed GMR energies of the Sn isotopes are lower than the values predicted by theoretical calculations that reproduce the GMR energies in 208Pb and 90Zr very well. From the GMR data, a value of Ktau = -550 +/- 100 MeV is obtained for the asymmetry term in the nuclear incompressibility. 相似文献
24.
Continuum generation from normally dispersive ultrahigh-numerical-aperture fibers deteriorates in relatively short times, limiting its application as a practical optical source for high-resolution optical coherence tomography. We find that reversible light-induced structural modification of fiber optic materials, rather than permanent optical damage, is responsible for this deterioration. By examining how the optical properties of corresponding light-induced waveguides depend on pumping wavelength, we isolate a waveguide that is beneficial for stable continuum generation. The performance deterioration due to the formation of other waveguides can be reversed by overwriting them with this particular waveguide. 相似文献
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Jerzy Chrusciel Krzysztof Matyjaszewski 《Journal of polymer science. Part A, Polymer chemistry》1996,34(11):2243-2252
Ring opening of 1,2,3,4-tetramethyl-1,2,3,4-tetraphenylcyclotetrasilane in the presence of various transition metal catalysts has been studied. Pd and Pt compounds are most active. Compounds with bulky ligands [e.g., Pd(PPh3)4] lead to the formation of “dimeric” cyclooctasilanes. Compounds with less bulky groups convert monomer to dimers and mixture of oligomers and polymers. Reactions with the all-trans monomer, tttt-(MePhSi)4, result in the formation of stereoregular dimer, presumably all-trans, tttttttt-(MePhSi)8, in high yields. Reactions in the presence of oxygen lead to the formation of polymers with inserted oxygen atoms in the main chain. © 1996 John Wiley & Sons, Inc. 相似文献
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Jerzy Król 《Foundations of Physics》2006,36(7):1070-1098
We analyse the proposition that the spacetime structure is modified at short distances or at high energies due to weakening of classical logic. The logic assigned to the regions of spacetime is intuitionistic logic of some topoi. Several cases of special topoi are considered. The quantum mechanical effects can be generated by such semi-classical spacetimes. The issues of: background independence and general relativity covariance, field theoretic renormalization of divergent expressions, the existence and definition of path integral measures, are briefly discussed in the proposal. The connection with some problems in foundations of mathematics and differential topology are also discussed. 相似文献
29.
Nash-Williams [6] formulated a condition that is necessary andsufficient for a countable family A=(Ai)iI of sets to have atransversal. In [7] he proved that his criterion applies alsowhen we allow the set I to be arbitrary and require only thatiJAi=Ø for any uncountable JI. In this paper, we formulateanother criterion of a similar nature, and prove that it isequivalent to the criterion of Nash-Williams for any familyu. We also present a self-contained proof that if iJAi=Øfor any uncountable JI, then our condition is necessary andsufficient for the family u to have a transversal. 相似文献
30.
Stanislav Dubniĉka Anna Zuzana Dubniĉkova Jerzy Kraskiewicz Ryszard Raczka 《Zeitschrift fur Physik C Particles and Fields》1995,68(1):153-162
The Körner-Kuroda model of the electromagnetic structure of octet 1/2+ baryons is restored on a more topical physical basis. Electromagnetic radii of baryons under consideration are calculated and compared with other model predictions. By an incorporation of a two-cut approximation of correct form factor analytic properties and nonzero vector-meson widths, the Körner-Kuroda model is unitarized, providing in this manner imaginary parts of the octet 1/2+ baryon form factors to be nonzero just starting from a branch point corresponding to the lowest threshold. 相似文献