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1.
Paul W. Percival 《Hyperfine Interactions》1991,65(1-4):901-911
As “rapporteur” for the papers submitted to this conference in the general area of muonium chemistry, I briefly review the
major developments since μSR86, and attempt to show how the papers presented at μSR90 relate to each other and work published
in the intervening years. Some topics are discussed in more detail than others, reflecting my own interests and views on what
is of current importance. Nevertheless, I try to cover all current research in muonium chemistry. The major areas are: early
events following muon thermalization, including subsequent loss of muon polarization (the “missing fraction”); molecular structure
and dynamics, primarily of muonium-substituted free radicals: and reaction kinetics. 相似文献
2.
3.
We describe a method for searching for ideal symmetric solutions to the Prouhet-Tarry-Escott Problem. We report results of extensive searches for solutions of sizes up to 12. We found two solutions of size 10 that are smaller by two orders of magnitude than the solution found by A. Letac in the 1940s, which was the smallest size 10 solution known before our search.
4.
Muon irradiation of pure liquid 3‐chloropropene, CH2=CH-CH2Cl, yields a primary radical, \dot\mboxCH2-CHMu-CH2Cl, and a secondary radical, MuCH2-\rm\dot\mboxCH-CH2Cl. 2‐methyl‐3‐chloropropene yields only the tertiary radical, MuCH2-\rm\dot\mboxC(CH3)-CH2Cl. These three chloroalkyl radicals have been characterized by μSR and μLCR, and the hyperfine coupling constants (hfcs)
have been determined over a range of temperatures, either in the pure liquid precursor or in concentrated solution. The temperature
variation of the hfcs has been analyzed to obtain estimates of the barrier to internal rotation about the C_\alpha-C_\beta
axis for various alkyl groups, and also their minimum energy conformations, i.e. their orientations with respect to the axis
of the 2p_z orbital of the unpaired electron. The tertiary radical is particularly interesting because all three methyl‐like
groups, -CH3,-CH2Cl and -CH2Mu, are represented. The results can be compared to electron spin resonance data for analogous radicals, to provide information
on the effects of Mu substitution for H.
This revised version was published online in August 2006 with corrections to the Cover Date. 相似文献
5.
Ghandi K Addison-Jones B Brodovitch JC McCollum BM McKenzie I Percival PW 《Journal of the American Chemical Society》2003,125(32):9594-9595
Muoniated free radicals have been detected in muon-irradiated aqueous solutions of acetone at high temperatures and pressures. At temperatures below 250 degrees C, the radical product is consistent with muonium addition to the keto form of acetone. However, at higher temperatures, a different radical was detected, which is attributed to muonium addition to the enol form. Muon hyperfine coupling constants have been determined for both radicals over a wide range of temperatures, significantly extending the range of conditions under which these radicals and the keto-enol equilibrium have been studied. 相似文献
6.
Deerenberg S Schrekker HS van Strijdonck GP Kamer PC van Leeuwen PW Fraanje J Goubitz K 《The Journal of organic chemistry》2000,65(16):4810-4817
A series of chiral phosphine-phosphite ligands 1-6 have been synthesized and used in the enantioselective palladium-catalyzed reaction of rac-1,3-diphenyl-2-propenyl acetate with dimethyl malonate as nucleophile. Ligands 1a, 2, 3, 5a, 6a, and 6b have been synthesized starting from racemic tert-butylphenylphosphinoborane. The use of dynamically resolved Li phosphide (-)-sparteine provided the optically pure ligands. Crystals of the allylpalladium (6a) complex were obtained, suitable for X-ray crystal structure determination. The X-ray crystal structure of the allylpalladium (6a) complex revealed a longer palladium-carbon bond distance trans to the phosphine moiety indicating that the attack of the nucleophile takes place at the carbon trans to the phosphine moiety. This was confirmed by the fact that the phosphine moiety did not affect the enantioselectivity directly. Under mild reaction conditions, enantioselectivities up to 83% were obtained (25 degrees C) with ligand 1e. Systematic variation of the ligand bridge and the phosphite moiety showed that the configuration of the product is controlled by the atropisomerism of the biphenyl substituent at the phosphite moiety. The conformation of the biphenyl group, in turn, is controlled by the substituent at the chiral carbon in the bridge. Ligands with large bite angles yielded higher enantioselectivities. 相似文献
7.
A computational study has been performed to examine the reactions of a model beta-diketiminatoaluminium (I) complex with the hydrogen atom and with the electron. It was found that the hydrogen atom adds to the metal centre exothermically (DeltaH(rxn)=-202 kJ mol(-1)), and the spin density in the resulting radical resides entirely on the beta-diketiminato ligand. The spin density of the corresponding radical anion is very similar to the H-adduct. 相似文献
8.
Feng Ji Paul W. Percival Jean-Claude Brodovitch Brenda Addison-Jones Stanislaw Wlodek 《Hyperfine Interactions》1994,87(1):853-858
Muonium adds to allyl chloride, CH2=CHCH2Cl, to form two radicals: MuCH2CHCH2Cl (main product) and CH2CHMuCH2Cl (minor product). Both radicals were fully characterized bySR andLCR. In the main product, the LCR lines due to the35Cl and37Cl nuclei were observed. Also, the temperature dependence of various hyperfine coupling constants (hfc) indicates that both Mu and Cl eclipse the unpaired electronp
2-orbital in the minimum energy conformation. For the fragment-CH2Cl, the presence of Mu in the-position is found to affect significantly the hfc of Cl in the-position; an internal rotational barrier of 12 kJ mol–1 was estimated using a simpleV
2 torsional potential. 相似文献
9.
Martina Schwager Emil Roduner Ivan D. Reid Paul W. Percival Jean-Claude Brodovitch Stanislaw Wlodek Robert F. Marzke 《Hyperfine Interactions》1994,87(1):859-864
SR spectra of the ethyl radical adsorbed on porous silica were observed in transverse and in longitudinal magnetic fields in the temperature range 190–298 K. The line widths reflect the dynamic partial averaging of the hyperfine anisotropy due to reorientation and surface diffusion. 相似文献
10.
Petra DG Kamer PC Spek AL Schoemaker HE van Leeuwen PW 《The Journal of organic chemistry》2000,65(10):3010-3017
A new class of efficient catalysts was developed for the asymmetric transfer hydrogenation of unsymmetrical ketones. A series of chiral N,S-chelates (6-22) was synthesized to serve as ligands in the iridium(I)-catalyzed reduction of ketones. Both formic acid and 2-propanol proved to be suitable as hydrogen donors. Sulfoxidation of an (R)-cysteine-based aminosulfide provided a diastereomeric ligand family containing a chiral sulfur atom. The two chiral centers of these ligands showed a clear effect of chiral cooperativity. In addition, aminosulfides containing two asymmetric carbon atoms in the backbone were synthesized. Both the sulfoxide-containing beta-amino alcohols and the aminosulfides derived from 1,2-disubstituted amino alcohols gave rise to high reaction rates and moderate to excellent enantioselectivities in the reduction of various ketones. The enantioselective outcome of the reaction was favorably affected by selecting the most appropriate hydrogen donor. Enantioselectivities of up to 97% were reached in the reduction of aryl-alkyl ketones. 相似文献