共查询到20条相似文献,搜索用时 15 毫秒
1.
Double CF Bond Activation through β‐Fluorine Elimination: Nickel‐Mediated [3+2] Cycloaddition of 2‐Trifluoromethyl‐1‐alkenes with Alkynes
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Tomohiro Ichitsuka Dr. Takeshi Fujita Tomohiro Arita Prof. Dr. Junji Ichikawa 《Angewandte Chemie (International ed. in English)》2014,53(29):7564-7568
The nickel‐mediated [3+2] cycloaddition of 2‐trifluoromethyl‐1‐alkenes with alkynes afforded fluorine‐containing multi‐substituted cyclopentadienes in a regioselective manner. This reaction involves the consecutive two C? F bond cleavage of a trifluoromethyl or a pentafluoroethyl group through β‐fluorine elimination. 相似文献
2.
Ni‐Catalyzed Synthesis of Fluoroarenes via [2+2+2] Cycloaddition Involving α‐Fluorine Elimination
下载免费PDF全文
![点击此处可从《Chemistry (Weinheim an der Bergstrasse, Germany)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Dr. Takeshi Fujita Yota Watabe Dr. Tomohiro Ichitsuka Prof.Dr. Junji Ichikawa 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(38):13225-13228
A method for direct synthesis of tetrasubstituted fluoroarenes via nickel‐catalyzed [2+2+2] cycloaddition is presented. The reaction combines one molecule of 1,1‐difluoroethylene with two molecules of alkynes and involves sequential cleavage of the C?F and C?H bonds in difluoroethylene. The catalytic cycle is established by reduction of the intermediary NiII fluoride with a triethylborane‐based borate. 相似文献
3.
4.
Cover Picture: Enantiospecific CH Activation Using Ruthenium Nanocatalysts (Angew. Chem. Int. Ed. 36/2015)
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Céline Taglang Luis Miguel Martínez‐Prieto Dr. Iker del Rosal Prof. Laurent Maron Prof. Romuald Poteau Dr. Karine Philippot Dr. Bruno Chaudret Dr. Serge Perato Anaïs Sam Lone Céline Puente Dr. Christophe Dugave Dr. Bernard Rousseau Dr. Grégory Pieters 《Angewandte Chemie (International ed. in English)》2015,54(36):10377-10377
5.
Synthesis of Silaphenalenes by Ruthenium‐Catalyzed Annulation between 1‐Naphthylsilanes and Internal Alkynes through CH Bond Cleavage
下载免费PDF全文
![点击此处可从《Chemistry (Weinheim an der Bergstrasse, Germany)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Dr. Yuichiro Tokoro Kengo Sugita Prof. Dr. Shin‐ichi Fukuzawa 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(38):13229-13232
Ruthenium‐catalyzed annulation of 1‐naphthylsilanes with internal alkynes afforded silaphenalenes through cleavage of the C?H bond at the 8‐position of the naphthalene. [RuH2(CO){P(p‐FC6H4)3}3] efficiently catalyzed the reaction. The use of 1‐naphthyldiphenylsilane as a substrate resulted in a better yield of the annulation product compared to the use of silanes with alkyl groups on the silicon atom. Internal alkynes with both aryl and alkyl groups were tolerated in this reaction. 相似文献
6.
Cover Picture: O2 Activation and Double CH Oxidation by a Mononuclear Manganese(II) Complex (Angew. Chem. Int. Ed. 2/2016)
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Dr. Claire Deville Sandeep K. Padamati Dr. Jonas Sundberg Prof. Dr. Vickie McKee Prof. Dr. Wesley R. Browne Prof. Dr. Christine J. McKenzie 《Angewandte Chemie (International ed. in English)》2016,55(2):453-453
7.
Inside Cover: Efficient Access to Titanaaziridines by CH Activation of N‐Methylanilines at Ambient Temperature (Angew. Chem. Int. Ed. 14/2015)
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Manfred Manßen Dr. Nicolai Lauterbach Jaika Dörfler Dr. Marc Schmidtmann Wolfgang Saak Prof. Dr. Sven Doye Prof. Dr. Rüdiger Beckhaus 《Angewandte Chemie (International ed. in English)》2015,54(14):4128-4128
8.
Rhodium(III)‐Catalyzed CC and CO Coupling of Quinoline N‐Oxides with Alkynes: Combination of CH Activation with O‐Atom Transfer
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Xueyun Zhang Zisong Qi Prof. Xingwei Li 《Angewandte Chemie (International ed. in English)》2014,53(40):10794-10798
[Cp*RhIII]‐catalyzed C? H activation of arenes assisted by an oxidizing N? O or N? N directing group has allowed the construction of a number of hetercycles. In contrast, a polar N? O bond is well‐known to undergo O‐atom transfer (OAT) to alkynes. Despite the liability of N? O bonds in both C? H activation and OAT, these two important areas evolved separately. In this report, [Cp*RhIII] catalysts integrate both areas in an efficient redox‐neutral coupling of quinoline N‐oxides with alkynes to afford α‐(8‐quinolyl)acetophenones. In this process the N? O bond acts as both a directing group for C? H activation and as an O‐atom donor. 相似文献
9.
Dipl.‐Chem. Inmaculada Mena Dr. Miguel A. Casado Dr. Víctor Polo Dr. Pilar García‐Orduña Prof. Fernando J. Lahoz Prof. Luis A. Oro 《Angewandte Chemie (International ed. in English)》2014,53(36):9627-9631
In the presence of phosphanes (PR3), the amido‐bridged trinuclear complex [{Ir(μ‐NH2)(tfbb)}3] (tfbb=tetrafluorobenzobarrelene) transforms into mononuclear discrete compounds [Ir(1,2‐η2‐4‐κ‐C12H8F4N)(PR3)3], which are the products of the C? N coupling between the amido moiety and a vinylic carbon of the diolefin. An alternative synthetic approach to these species involves the reaction of the 18 e? complex [Ir(Cl)(tfbb)(PMePh2)2] with gaseous ammonia and additional phosphane. DFT studies show that both transformations occur through nucleophilic attack. In the first case the amido moiety attacks a diolefin coordinated to a neighboring molecule following a bimolecular mechanism induced by the highly basic NH2 moiety; the second pathway involves a direct nucleophilic attack of ammonia to a coordinated tfbb molecule. 相似文献
10.
Nickel‐Catalyzed Chemo‐, Regio‐ and Diastereoselective Bond Formation through Proximal CC Cleavage of Benzocyclobutenones
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Dr. Francisco Juliá‐Hernández Dr. Asraa Ziadi Dr. Akira Nishimura Prof. Ruben Martin 《Angewandte Chemie (International ed. in English)》2015,54(33):9537-9541
The first catalytic intermolecular proximal C1? C2 cleavage of benzocyclobutenones (BCB) without prior carbonyl activation or employing noble metals has been developed. This protocol operates at room temperature and is characterized by an exquisite chemo‐, regio‐ and diastereoselectivity profile, constituting a unique platform for preparing an array of elusive carbocyclic skeletons. 相似文献
11.
Manganese‐Catalyzed Dehydrogenative [4+2] Annulation of NH Imines and Alkynes by CH/NH Activation
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Ruoyu He Prof. Dr. Zhi‐Tang Huang Prof. Dr. Qi‐Yu Zheng Prof. Dr. Congyang Wang 《Angewandte Chemie (International ed. in English)》2014,53(19):4950-4953
Described herein is a manganese‐catalyzed dehydrogenative [4+2] annulation of N? H imines and alkynes, a reaction providing highly atom‐economical access to diverse isoquinolines. This transformation represents the first example of manganese‐catalyzed C? H activation of imines; the stoichiometric variant of the cyclomanganation was reported in 1971. The redox neutral reaction produces H2 as the major byproduct and eliminates the need for any oxidants, external ligands, or additives, thus standing out from known isoquinoline synthesis by transition‐metal‐catalyzed C? H activation. Mechanistic studies revealed the five‐membered manganacycle and manganese hydride species as key reaction intermediates in the catalytic cycle. 相似文献
12.
Dr. Rishikesh Narayan Dr. Kiran Matcha Dr. Andrey P. Antonchick 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(42):14678-14693
The formation of C?C bonds embodies the core of organic chemistry because of its fundamental application in generation of molecular diversity and complexity. C?C bond‐forming reactions are well‐known challenges. To achieve this goal through direct functionalization of C?H bonds in both of the coupling partners represents the state‐of‐the‐art in organic synthesis. Oxidative C?C bond formation obviates the need for prefunctionalization of both substrates. This Minireview is dedicated to the field of C?C bond‐forming reactions through direct C?H bond functionalization under completely metal‐free oxidative conditions. Selected important developments in this area have been summarized with representative examples and discussions on their reaction mechanisms. 相似文献
13.
Nagaraju Barsu Deepti Kalsi Prof. Basker Sundararaju 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(26):9364-9368
A one‐step synthetic method was developed for allylation of benzamides using Ni(COD)2/RCO2H and [Ni(μ‐H2O)(OOCCMe3)2(HOOCCMe3)2]2 ( A′ ) catalytic system. Efficient, well‐defined, air and moisture‐stable Ni–pivalate complex was isolated and employed in catalytic allylation. The influence of solvent on product selectivity was also investigated. 相似文献
14.
15.
Dr. Margaret L. Scheuermann David W. Boyce Prof. Kyle A. Grice Prof. Werner Kaminsky Prof. Stefan Stoll Prof. William B. Tolman Prof. Ole Swang Prof. Karen I. Goldberg 《Angewandte Chemie (International ed. in English)》2014,53(25):6492-6495
[Pd(P(Ar)(tBu)2)2] ( 1 , Ar=naphthyl) reacts with molecular oxygen to form PdII hydroxide dimers in which the naphthyl ring is cyclometalated and one equivalent of phosphine per palladium atom is released. This reaction involves the cleavage of both C? H and O? O bonds, two transformations central to catalytic aerobic oxidizations of hydrocarbons. Observations at low temperature suggest the initial formation of a superoxo complex, which then generates a peroxo complex prior to the C? H activation step. A transition state for energetically viable C? H activation across a Pd? peroxo bond was located computationally. 相似文献
16.
Hui Yu Guoying Zhang Prof. Dr. Hanmin Huang 《Angewandte Chemie (International ed. in English)》2015,54(37):10912-10916
A fundamentally novel approach to bioactive quinolizinones is based on the palladium‐catalyzed intramolecular cyclocarbonylation of allylamines. [Pd(Xantphos)I2], which features a very large bite angle, has been found to facilitate the rapid carbonylation of azaarene‐substituted allylamines into bioactive quinolizinones in good to excellent yields. This transformation represents the first dearomative carbonylation and is proposed to proceed by palladium‐catalyzed C? N bond activation, dearomatization, CO insertion, and a Heck reaction. 相似文献
17.
Lewis Acid Mediated Tandem Reaction of Propargylic Alcohols to Tetrazoles Involving CO‐ and CC‐Bond Cleavage Reactions and a CN‐Bond Formation
下载免费PDF全文
![点击此处可从《Chemistry (Weinheim an der Bergstrasse, Germany)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Dr. Xian‐Rong Song Ya‐Ping Han Yi‐Feng Qiu Zi‐Hang Qiu Xue‐Yuan Liu Prof. Dr. Peng‐Fei Xu Prof. Dr. Yong‐Min Liang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(38):12046-12050
A novel and direct synthesis of 1‐aryl‐5‐arylvinyl‐tetrazoles from easily prepared propargylic alcohols and TMSN3 is developed in the presence of TMSCl under mild conditions (TMS=trimethylsilyl). The process involves an allenylazide intermediate, followed by a C?C‐bond cleavage and C?N‐bond formation to afford the desired products. Moreover, this method offers a good functional‐group applicability and can be scaled‐up to grams (yield up to 85 %). 相似文献
18.
Mechanistic Study on Rh‐Catalyzed Stereoselective CC/CH Activation of tert‐Cyclobutanols
下载免费PDF全文
![点击此处可从《Chemistry (Weinheim an der Bergstrasse, Germany)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Dr. Haizhu Yu Dr. Chen Wang Yimeng Yang Prof. Zhi‐Min Dang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(13):3839-3848
A mechanistic study was performed on the Rh‐catalyzed stereoselective C?C/C?H activation of tert‐cyclobutanols. The present study corroborated the previous proposal that the reaction occurs by metalation, β‐C elimination, 1,4‐Rh transfer, C?O insertion, and a final catalyst‐regeneration step. The rate‐determining step was found to be the 1,4‐Rh transfer step, whereas the stereoselectivity‐determining step did not correspond to any of the aforementioned steps. It was found that both the thermodynamic stability of the product of the β‐C elimination and the kinetic feasibility of the 1,4‐Rh transfer and C?O insertion steps made important contributions. In other words, three steps (i.e., β‐C elimination, 1,4‐Rh transfer, and C?O insertion) were found to be important in determining the configurations of the two quaternary stereocenters. 相似文献
19.
Tomohiro Ichitsuka Takeshi Fujita Tomohiro Arita Junji Ichikawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2014,126(29):7694-7698
The nickel‐mediated [3+2] cycloaddition of 2‐trifluoromethyl‐1‐alkenes with alkynes afforded fluorine‐containing multi‐substituted cyclopentadienes in a regioselective manner. This reaction involves the consecutive two C F bond cleavage of a trifluoromethyl or a pentafluoroethyl group through β‐fluorine elimination. 相似文献
20.
Ke Yang Cheng Zhang Peng Wang Prof. Dr. Yan Zhang Prof. Dr. Haibo Ge 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(24):7241-7244
Nickel‐catalyzed ligand‐free decarboxylative cross‐coupling of azole derivatives with α‐oxoglyoxylic acids has been developed. This work represents the first example of decarboxylative cross‐coupling reactions, in a C?H bond functionalization manner, through nickel catalysis, and tolerates various functional groups. Additionally, this approach provides an efficient access to azole ketones, an important structural motif in many medicinal compounds with a broad range of biological activities. 相似文献