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Oxidative Addition of Haloheteroarenes to Palladium(0): Concerted versus SNAr‐Type Mechanism
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Prof. Bert U. W. Maes Dr. Stefan Verbeeck Dr. Tom Verhelst Audrey Ekomié Niklas von Wolff Dr. Guillaume Lefèvre Dr. Emily A. Mitchell Prof. Anny Jutand 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(21):7858-7865
The kinetics of the oxidative additions of haloheteroarenes HetX (X=I, Br, Cl) to [Pd0(PPh3)2] (generated from [Pd0(PPh3)4]) have been investigated in THF and DMF and the rate constants have been determined. In contrast to the generally accepted concerted mechanism, Hammett plots obtained for substituted 2‐halopyridines and solvent effects reveal a reaction mechanism dependent on the halide X of HetX: an unprecedented SNAr‐type mechanism for X=Br or Cl and a classical concerted mechanism for X=I. These results are supported by DFT studies. 相似文献
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Niklas Jänsch Wisely Oki Sugiarto Marius Muth Aleksandra Kopranovic Charlotte Desczyk Matthias Ballweg Frank Kirschhöfer Dr. Gerald Brenner-Weiss Prof. Dr. Franz-Josef Meyer-Almes 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(58):13249-13255
Human histone deacetylase 8 is a well-recognized target for T-cell lymphoma and particularly childhood neuroblastoma. PD-404,182 was shown to be a selective covalent inhibitor of HDAC8 that forms mixed disulfides with several cysteine residues and is also able to transform thiol groups to thiocyanates. Moreover, HDAC8 was shown to be regulated by a redox switch based on the reversible formation of a disulfide bond between cysteines Cys102 and Cys153. This study on the distinct effects of PD-404,182 on HDAC8 reveals that this compound induces the dose-dependent formation of intramolecular disulfide bridges. Therefore, the inhibition mechanism of HDAC8 by PD-404,182 involves both, covalent modification of thiols as well as ligand mediated disulfide formation. Moreover, this study provides a deep molecular insight into the regulation mechanism of HDAC8 involving several cysteines with graduated capability to form reversible disulfide bridges. 相似文献
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Jared M. Schwartz Oluwadamilola Phillips Anthony Engler Alexandra Sutlief Jihyun Lee Paul A. Kohl 《Journal of polymer science. Part A, Polymer chemistry》2017,55(7):1166-1172
Low ceiling temperature, thermodynamically unstable polymers have been troublesome to synthesize and keep stable during storage. In this study, stable poly(phthalaldehyde) has been synthesized with BF3‐OEt2 catalyst. The role of BF3 in the polymerization is described. The interaction of BF3 with the monomer is described and used to maximize the yield and molecular weight of poly(phthalaldehyde). Various Lewis acids were used to investigate the effect of catalyst acidity on poly(phthalaldehyde) chain growth. In situ nuclear magnetic resonance was used to identify possible interactions formed between BF3 and phthalaldehyde monomer and polymer. The molecular weight of the polymer tracks with polymerization yield. The ambient temperature stability of poly(phthalaldehyde) was investigated and the storage life of the polymer has been improved. © 2016 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2016 , 55, 1166–1172 相似文献
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Dimesitylmethane-based compounds 9–17, incorporating four groups capable of serving as hydrogen bonding sites, such as pyrazole, pyrimidine, imidazole, indole and aminoalkyl groups, were prepared and their ability to complex selected carbohydrates tested. The tetrasubstituted dimesitylmethane scaffold provides a cavity of a correct shape and size for disaccharide encapsulation and its aromatic units are able to participate in CH-π interactions with the sugar substrate. First binding studies confirmed the expected di- vs monosaccharide binding preference of this type of compounds and their tendency to form strong complexes with maltoside. 相似文献
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Jens Rudlof Niklas Aders Dr. Jan-Hendrik Lamm Beate Neumann Dr. Hans-Georg Stammler Prof. Dr. Norbert W. Mitzel 《ChemistryOpen》2021,10(10):1020-1027
Starting from 1,2-diethynylbenzene, a series of bidentate Lewis acids was prepared by means of hydrometalations, in particular hydrosilylation, hydroboration, hydroalumination and terminal metalation based on group 13 and 14 elements. In the case of terminal alkyne metalation, the Lewis-acidic gallium function was introduced using triethylgallium under alkane elimination. A total of six different Lewis acids based on a semiflexible organic scaffold were prepared, bearing −SiClMe2, −SiCl2Me, −SiCl3, −B(C6F5)2, −AlBis2 (Bis=bis(trimethylsilyl)methyl) and −GaEt2 as the corresponding functional units. In all cases, the Lewis acid functionalisation was carried out twice and the products were obtained in good to excellent yields. In the case of the twofold gallium Lewis acid, a different structural motif in the form of a polymer-like chain was observed in the solid state. All new bidentate Lewis acids were characterised by multinuclear NMR spectroscopy, CHN analysis and X-ray diffraction experiments. 相似文献