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Wang Wang Chao Ding Yangyang Li Zheqi Li Yuqiang Li Long Peng Guoyin Yin 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(14):4660-4664
An unprecedented arylboration of unactivated terminal alkenes, featuring 1,n‐regioselectivity, has been achieved by nickel catalysis. The nitrogen‐based ligand plays an essential role in the success of this three‐component reaction. This transformation displays good regioselectivity and excellent functional‐group tolerance. In addition, the incorporation of a boron group into the products provides substantial opportunities for further transformations. Also demonstrated is that the products can be readily transformed into pharmaceutically relevant molecules. Unexpectedly, preliminary mechanistic studies indicate that although the metal migration favors the α‐position of boron, selective and decisive bond formation is favored at the benzylic position. 相似文献
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Tingshun Zhu Yingguo Liu Marie Smetankova Shitian Zhuo Chengli Mou Huifang Chai Zhichao Jin Yonggui Robin Chi 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(44):15925-15929
Multisubstituted arenes such as indanes with attached all‐carbon quaternary centers are unique scaffolds in synthetic functional molecules and sophisticated natural products. A key challenge in preparing such molecules lies in the enantioselective installation of the quaternary carbon centers. Conventional methods in this direction include asymmetric substitution reactions and substrate‐controlled cyclization reactions. These reactions lead to poor stereoselectivities and/or require long and tedious synthetic steps. Disclosed here is a one‐step organic catalytic strategy for enantioselective access to this class of molecules. The reaction involves an N‐heterocyclic carbene catalyzed process for direct benzene construction, indane formation, remote‐carbon desymmetrization, and excellent chirality control. This approach will enable the concise synthesis of arene‐containing molecules, including those with complex structures and challenging chiral centers. 相似文献
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Simon M. Nicolle William Lewis Christopher J. Hayes Christopher J. Moody 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2015,127(29):8605-8609
Copper‐ or rhodium‐catalyzed reactions of diazocarbonyl compounds with β‐hydroxyketones give highly substituted tetrahydrofurans with excellent diastereoselectivity. Under mild conditions, the single‐step process starts as a carbene O H insertion reaction, but is diverted by an intramolecular aldol reaction. 相似文献
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Wen‐Hao Li Cun‐Yao Li Huan‐Yan Xiong Yang Liu Wen‐Yong Huang Guang‐Jun Ji Zheng Jiang Hai‐Tao Tang Ying‐Ming Pan Yun‐Jie Ding 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(8):2470-2475
Heterogeneous, metal, single‐site catalysts often exhibit higher catalytic performance than other catalysts because of their maximized atom efficiency of 100 %. Reported herein is a precoordination/solvothermal polymerization strategy to fabricate a stable mononuclear Pd‐metalized porous organic polymer catalyst (Pd@POP). Pd@POP was easy to use in regioselective organic reactions because the internal structure of this Pd@POP can be easily modified. The catalyst was used to solve the intractable regioselectivity problems of Heck reactions. Pd@POP‐9 can efficiently activate the ends of olefins, thereby leading to high selectivity for substitution at the external position. To understand the reason underlying the high selectivity and activity of the catalyst, the systemic characterization of Pd@POP‐9 and density‐functional theory calculations were conducted. This Heck reaction is the first to be catalyzed by a recyclable mononuclear metal catalyst with unprecedented catalytic activity and regioselectivity. 相似文献
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Ya Chen Yixiao Pan Yan‐Mei He Qing‐Hua Fan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(47):16987-16990
A highly enantioselective iridium‐ or ruthenium‐catalyzed intermolecular reductive amination/asymmetric hydrogenation relay with 2‐quinoline aldehydes and aromatic amines has been developed. A broad range of sterically tunable chiral N,N′‐diaryl vicinal diamines were obtained in high yields (up to 95 %) with excellent enantioselectivity (up to >99 % ee). The resulting chiral diamines could be readily transformed into sterically hindered chiral N‐heterocyclic carbene (NHC) precursors, which are otherwise difficult to access. The usefulness of this synthetic approach was further demonstrated by the successful application of one of the chiral vicinal diamines and chiral NHC ligands in a transition‐metal‐catalyzed asymmetric Suzuki–Miyaura cross‐coupling reaction and asymmetric ring‐opening cross‐metathesis, respectively. 相似文献
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Nicolas Blanchard Vincent Bizet 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(21):6886-6889
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Michal S. Shoshan Thomas Vonderach Bodo Hattendorf Helma Wennemers 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(15):4955-4959
Peptide‐stabilized platinum nanoparticles (PtNPs) were developed that have significantly greater toxicity against hepatic cancer cells (HepG2) than against other cancer cells and non‐cancerous liver cells. The peptide H‐Lys‐Pro‐Gly‐d Lys‐NH2 was identified by a combinatorial screening and further optimized to enable the formation of water‐soluble, monodisperse PtNPs with average diameters of 2.5 nm that are stable for years. In comparison to cisplatin, the peptide‐coated PtNPs are not only more toxic against hepatic cancer cells but have a significantly higher tumor cell selectivity. Cell viability and uptake studies revealed that high cellular uptake and an oxidative environment are key for the selective cytotoxicity of the peptide‐coated PtNPs. 相似文献
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