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The intricacies of the synthetic chemistry executed by living cells in the assembly of complex organic natural products can be probed in great detail by stable-isotope labeling in conjunction with sophisticated 2D and multiple-quantum NMR methods of analysis. Mechanistic details are revealed by unraveling the “cryptic” stereochemistry of biosynthetic reactions with the aid of stereospecific isotope labeling. Analysis of blocked mutants and cloning of biosynthetic genes provides new tools for the study of biosynthetic pathways and for the exploitation of the chemical capabilities of living organisms. 相似文献
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Grandjean D Beale AM Petukhov AV Weckhuysen BM 《Journal of the American Chemical Society》2005,127(41):14454-14465
The hydrothermal crystallization of CoAPO-5 molecular sieves has been studied using time-resolved in-situ SAXS/WAXS, UV-vis, Raman, and XAS. Data collected during heating to 180 degrees C allowed the observation of different steps occurring during the transformation of the amorphous gel into a crystalline material from a macroscopic and atomic perspective. Raman spectroscopy detected the initial formation of Al-O-P bonds, whereas SAXS showed that these gel particles had a broad size distribution ranging from ca. 7 to 20 nm before crystallization began. WAXS showed that this crystallization was sharp and occurred at around 160 degrees C. Analysis of the crystallization kinetics suggested a one-dimensional growth process. XAS showed that Co(2+) transformed via a two-stage process during heating involving (i) a gradual transformation of octahedral coordination into tetrahedral coordination before the appearance of Bragg peaks corresponding to AFI, suggesting progressive incorporation of Co(2+) into the poorly ordered Al-O-P network up to ca. 150 degrees C, and (ii) a rapid transformation of remaining octahedral Co(2+) at the onset of crystallization. Co(2+) was observed to retard crystallization of AFI but provided valuable information regarding the synthesis process by acting as an internal probe. A three-stage, one-dimensional crystallization mechanism is proposed: (i) an initial reaction between aluminum and phosphate units forming a primary amorphous phase, (ii) progressive condensation of linear Al-O-P chains forming a poorly ordered structure separated by template molecules up to ca. 155 degrees C, and (iii) rapid internal reorganization of the aluminophosphate network leading to crystallization of the AFI crystal structure. 相似文献
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Summary This paper adds the finishing touches to an algorithmic treatment of quadratic forms over the rational numbers. The Witt index of a rational quadratic form is explicitly computed. When combined with a recent adjustment in the Haase invariants, this gives a complete set of invariants for rational quadratic forms, a set which can be computed and which respects all of the standard natural operations (including the tensor product) for quadratic forms. The overall approach does not use (at least explicitly) anyp-adic methods, but it does give the Witt ring of thep-adics as well as the Witt ring of the rationals. 相似文献
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G.R. Hyde R.O. Dillon H.A. Beale I.L. Spain J.A. Woollam David J. Sellmyer 《Solid State Communications》1973,13(3):257-263
Shubnikov-de Haas frequencies were measured in highly degenerate n-type Bi2Se3 having a higher carrier density (~9 × 1025m-3) than previously reported. The Fermi surface was found to be elongated along the trigonal axis, fitting a spheroidal model with an axial ratio of 5.0 for angles up to θ = 45°. Comparison of the number of carriers obtained from Hall measurements with that obtained from the Shubnikov-de Haas measurement supports the contention that the lowest conduction band minimum is a single surface located in the center of the Brillouin zone. The higher effective mass (0.25 m0) found for these carrier concentrations indicates that the band is non-parabolic. 相似文献
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Beale 《Fresenius' Journal of Analytical Chemistry》1862,1(1):264
Ohne Zusammenfassung 相似文献
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Abazov VM Abbott B Acharya BS Adams M Adams T Alexeev GD Alkhazov G Alton A Alverson G Alves GA Aoki M Arov M Askew A Asman B Atramentov O Avila C Backusmayes J Badaud F Bagby L Baldin B Bandurin DV Banerjee S Barberis E Baringer P Barreto J Bartlett JF Bassler U Bazterra V Beale S Bean A Begalli M Begel M Belanger-Champagne C Bellantoni L Beri SB Bernardi G Bernhard R Bertram I Besançon M Beuselinck R Bezzubov VA Bhat PC Bhatnagar V Blazey G Blessing S Bloom K Boehnlein A Boline D Boos EE 《Physical review letters》2011,107(1):011804
We present a study of the dijet invariant mass spectrum in events with two jets produced in association with a W boson in data corresponding to an integrated luminosity of 4.3 fb(-1) collected with the D0 detector at √s = 1.96 TeV. We find no evidence for anomalous resonant dijet production and derive upper limits on the production cross section of an anomalous dijet resonance recently reported by the CDF Collaboration, investigating the range of dijet invariant mass from 110 to 170 GeV/c(2). The probability of the D0 data being consistent with the presence of a dijet resonance with 4 pb production cross section at 145 GeV/c(2) is 8×10(-6). 相似文献