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Steven S. Wesolowski Edward F. Valeev Rollin A. King Victor Baranovski Henry F. Schaefer III 《Molecular physics》2013,111(16):1227-1231
Atomic natural orbital (ANO) basis sets for calcium may produce surprisingly poor atomic and molecular properties and energetics. The weaknesses in these basis sets may be traced primarily to deficiencies within the sets of d functions which are incapable of effectively correlating the 3s and 3p electrons. Examples are given which show that addition of tight d functions to the ANO basis is required to achieve qualitatively correct energetics and structures for conventionally bonded calcium compounds. 相似文献
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The gas‐phase pyrolytic and oxidative chemistry of furans has received much attention recently because of their potential as platform chemicals and biofuels. Typically these compounds exhibit very strong ring carbon to H or CH3 bonds. 2‐Methoxyfuran had been reported to be exceptionally unstable in comparison to related substituted heterocycles in pyrolytic experiments. The origins of its reactivity are shown to be due to the very weak O–CH3, which at 189.5 ± 1.9 kJ mol?1 is some 200 kJ mol?1 weaker than C–H bonds in the molecule. We show that the reported reactivity is somewhat overestimated but that does not alter the fact that 2‐methoxyfuran is exceptionally unstable. It may prove to be a useful alternative to azomethane as a thermal source of methyl radicals. 相似文献
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Electrochemical Vicinal Difluorination of Alkenes: Scalable and Amenable to Electron-Rich Substrates
Sayad Doobary Alexi T. Sedikides Henry P. Caldora Dr. Darren L. Poole Dr. Alastair J. J. Lennox 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(3):1171-1176
Fluorinated alkyl groups are important motifs in bioactive compounds, positively influencing pharmacokinetics, potency and conformation. The oxidative difluorination of alkenes represents an important strategy for their preparation, yet current methods are limited in their alkene-types and tolerance of electron-rich, readily oxidized functionalities, as well as in their safety and scalability. Herein, we report a method for the difluorination of a number of unactivated alkene-types that is tolerant of electron-rich functionality, giving products that are otherwise unattainable. Key to success is the electrochemical generation of a hypervalent iodine mediator using an “ex-cell” approach, which avoids oxidative substrate decomposition. The more sustainable conditions give good to excellent yields in up to decagram scales. 相似文献
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J. D. Henry Jr. M. E. Prudich K. R. Vaidyanathan 《Separation & Purification Reviews》2013,42(2):81-118
The removal of the mineral matter found in coal derived liquids is a very difficult solid/liquid separation process. Clays, pyrites and other minerals that occur in coal ultimately find their way into the liquefied product. This is the case, e.g., for both the solvent refined coal (SRC-I) and H-Coal processes. The ash content of bituminous coals which may be fed to coal liquefaction processes normally rangesfrom 6 to 11 wt.%. The ash content of the coal liquid product can range from 4 to 20 wt.% depending upon the lique-faction .process. Ash levels must be reduced to, e.g., 0.4 wt.% in the case of boiler fuel and less than 0.1 wt.% for gas turbine fuels. 相似文献