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111.
Mixed‐Metal MIL‐100(Sc,M) (M=Al,Cr, Fe) for Lewis Acid Catalysis and Tandem CC Bond Formation and Alcohol Oxidation 下载免费PDF全文
Laura Mitchell Patrick Williamson Barbora Ehrlichová Amanda E. Anderson Valerie R. Seymour Sharon E. Ashbrook Nadia Acerbi Luke M. Daniels Richard I. Walton Matthew L. Clarke Paul A. Wright 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(51):17185-17197
The trivalent metal cations Al3+, Cr3+, and Fe3+ were each introduced, together with Sc3+, into MIL‐100(Sc,M) solid solutions (M=Al, Cr, Fe) by direct synthesis. The substitution has been confirmed by powder X‐ray diffraction (PXRD) and solid‐state NMR, UV/Vis, and X‐ray absorption (XAS) spectroscopy. Mixed Sc/Fe MIL‐100 samples were prepared in which part of the Fe is present as α‐Fe2O3 nanoparticles within the mesoporous cages of the MOF, as shown by XAS, TGA, and PXRD. The catalytic activity of the mixed‐metal catalysts in Lewis acid catalysed Friedel–Crafts additions increases with the amount of Sc present, with the attenuating effect of the second metal decreasing in the order Al>Fe>Cr. Mixed‐metal Sc,Fe materials give acceptable activity: 40 % Fe incorporation only results in a 20 % decrease in activity over the same reaction time and pure product can still be obtained and filtered off after extended reaction times. Supported α‐Fe2O3 nanoparticles were also active Lewis acid species, although less active than Sc3+ in trimer sites. The incorporation of Fe3+ into MIL‐100(Sc) imparts activity for oxidation catalysis and tandem catalytic processes (Lewis acid+oxidation) that make use of both catalytically active framework Sc3+ and Fe3+. A procedure for using these mixed‐metal heterogeneous catalysts has been developed for making ketones from (hetero)aromatics and a hemiacetal. 相似文献
112.
McCarron P Emteborg H Giddings SD Wright E Quilliam MA 《Analytical and bioanalytical chemistry》2011,400(3):847-858
A candidate certified reference material (CRM) for multiple shellfish toxins (domoic acid, okadaic acid and dinophysistoxins,
pectenotoxins, yessotoxin, azaspiracids and spirolides) has been prepared as a freeze-dried powder from mussel tissues (Mytilus edulis). Along with the certified values, the most important characteristics for a reference material to be fit-for-purpose are
homogeneity and stability. Acceptable between-bottle homogeneity was found for this CRM. Within-bottle homogeneity was assessed
using domoic acid, and it was shown that repeated subsampling of the CRM can be performed precisely down to 0.35 g. Both short-
and long-term stability studies carried out under isochronous conditions demonstrated excellent stability of the various toxins
present in the material. While degradation of some analytes was observed at +60°C in short-term studies, it was determined
that shipping at ambient temperature is adequate. No instability was detected in long-term stability studies, and it was shown
that the material can be held at +18°C safely for up to 1 year. To guarantee stability of the CRM over its lifetime the stock
will be maintained at −20°C. The results of the homogeneity and stability testing show that CRM–FDMT1 is appropriate for its
intended use in quality assurance and quality control of shellfish toxin analysis methods. 相似文献
113.
A key contact in the active site of an aminoglycoside phosphotransferase enzyme (APH(3')-IIIa) is a pi-pi stacking interaction between Tyr42 and the adenine ring of bound nucleotides. We investigated the prevalence of similar Tyr-adenine contacts and found that many different protein systems employ Tyr residues in the recognition of the adenine ring. The geometry of these stacking interactions suggests that electrostatics play a role in the attraction between these aromatic systems. Kinetic and calorimetric experiments on wild-type and mutant forms of APH(3')-IIIa yielded further experimental evidence of the importance of electrostatics in the adenine binding region and suggested that the stacking interaction contributes approximately 2 kcal/mol of binding energy. This type of information concerning the forces that govern nucleotide binding in APH(3')-IIIa will facilitate inhibitor design strategies that target the nucleotide binding site of APH-type enzymes. 相似文献
114.
Bearman KR Blackmore DC Carter TJ Colin F Wright JD Ross SA 《Chemical communications (Cambridge, England)》2002,(9):980-981
Encapsulation of Amberlyst A-26 supported tribromide in a 10,000 MW polyethylene glycol matrix gives a robust colour-sensitive reagent matrix which can be deposited on indium-tin oxide coated polyvinylidene fluoride (PVDF) piezoelectric film for the detection of styrene (and other alkene) vapours. 相似文献
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Tripathi S Armstrong DS Christy ME Clark JH Gorringe TP Hasinoff MD Kovash MA Wright DH Zołnierczuk PA 《Physical review letters》2002,89(25):252501
We report the first observation of double radiative capture on pionic hydrogen. The experiment was conducted at the TRIUMF cyclotron using the RMC spectrometer and detected gamma-ray coincidences following pi(-) stops in liquid hydrogen. We found the branching ratio for double radiative capture to be [3.05+/-0.27(stat)+/-0.31(syst)]x10(-5). The measured branching ratio and angle-energy distributions support the theoretical prediction of a dominant contribution from the pipi-->gammagamma annihilation mechanism. 相似文献
118.
We develop a variational theory of the crossover from the one-dimensional (1D) regime to the 3D regime for ultracold Bose gases in thin waveguides. Within the 1D regime we map out the parameter space for fermionization, which may span the full 1D regime for suitable transverse confinement. 相似文献
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