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Benjamin D. A. Shennan Peter W. Smith Yusuke Ogura Darren J. Dixon 《Chemical science》2020,11(38):10354
An efficient three-step sequence to afford a valuable class of spirocyclic pyrrolidines is reported. A reductive cleavage/Horner–Wadsworth–Emmons cascade facilitates the spirocyclisation of a range of isoxazolines bearing a distal β-ketophosphonate. The spirocyclisation precursors are elaborated in a facile and modular fashion, via a [3 + 2]-cycloaddition followed by the condensation of a phosphonate ester, introducing multiple points of divergence. The synthetic utility of this protocol has been demonstrated in the synthesis of a broad family of 1-azaspiro[4,4]nonanes and in a concise formal synthesis of the natural product (±)-cephalotaxine.A three-step, modular and divergent sequence accessing challenging spirocyclic pyrrolidines has been developed, featuring a novel reductive spirocyclization cascade. 相似文献
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The radiation-induced emulsion copolymerization of tetrafluoroethylene with propylene was carried out at room temperature in the presence of gaseous monomers. The formation of hydrofluoric acid in the course of polymerization was observed. The amount of HF formed increased linearly with the irradiation time at various dose rates in the early stage. The tendency was similar to that of time-polymer yield curves. The rate of HF formation was proportional to the first order of the dose rate. The amount of HF formed increased in the presence of oxygen and decreased remarkably above 1 wt% emulsifier, while the polymer yield decreased in the presence of oxygen and increased with the emulsifier concentration. A remarkable decrease in the amount of HF formed in higher emulsifier concentration is mainly attributable to chemical absorption or electrostatic capture of H+ ion on polymer particles produced. Hydrofluoric acid is mainly formed by reaction between primary products (e aq ? and H) from the radiolysis of water and organic fluoride (tetrafluoroethylene and emulsifier), and is little formed by reaction between primary products and copolymer produced. The G value of HF formation was in the order of emulsifier-water system > suspension polymerization > emulsion polymerization, while the polymer yield was in the order of emulsion polymerization > suspension polymerization. 相似文献
5.
Yoshio Aso Shoji Nishiguchi Tetsuya Jigami Tetsuo Otsubo Fumio Ogura 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1):417-418
Several well-defined 3,4-thienylene-ethynylene oligomers with different chain lengths have been synthesized and characterized. X-Ray crystallographic analyses proved their unique, totally helical conformations. 相似文献
6.
Jie Zhu Dr. Ryota Osuga Prof. Ryo Ishikawa Prof. Naoya Shibata Prof. Yuichi Ikuhara Prof. Junko N. Kondo Prof. Masaru Ogura Prof. Jihong Yu Prof. Toru Wakihara Prof. Zhendong Liu Prof. Tatsuya Okubo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(44):19837-19842
Encapsulating metal nanoclusters into zeolites combines the superior catalytic activity of the nanoclusters with high stability and unique shape selectivity of the crystalline microporous materials. The preparation of such bifunctional catalysts, however, is often restricted by the mismatching in time scale between the fast formation of nanoclusters and the slow crystallization of zeolites. We herein demonstrate a novel strategy to overcome the mismatching issue, in which the crystallization of zeolites is expedited so as to synchronize it with the rapid formation of nanoclusters. The concept was demonstrated by confining Pt and Sn nanoclusters into a ZSM-5 (MFI) zeolite in the course of its crystallization, leading to an ultrafast, in situ encapsulation within just 5 min. The Pt/Sn-ZSM-5 exhibited exceptional activity and selectivity with stability in the dehydrogenation of propane to propene. This method of ultrafast encapsulation opens up a new avenue for designing and synthesizing composite zeolitic materials with structural and compositional complexity. 相似文献
7.
Total Synthesis of the Antibiotic Kendomycin: A Macrocyclization Using the Tsuji–Trost Etherification 下载免费PDF全文
Dr. Tetsuya Sengoku Dr. Shu Xu Kenji Ogura Yoshinori Emori Kenji Kitada Prof. Dr. Daisuke Uemura Prof. Dr. Hirokazu Arimoto 《Angewandte Chemie (International ed. in English)》2014,53(16):4213-4216
A highly stereocontrolled, convergent total synthesis of kendomycin [(?)‐TAN2162], an ansa‐macrocyclic antibiotic, is reported. The key of the strategy is an unprecedented Tsuji–Trost macrocyclic etherification, followed by a transannular Claisen rearrangement to construct the 18‐membered carbocyclic framework. The oxa‐six‐ and five‐membered rings were also stereoselectively constructed respectively by a cascade oxidative cyclization at an unfunctionalized benzylic position and using a one‐pot epoxidation/5‐exo‐tet epoxide opening. 相似文献
8.
Raku Watanabe Dr. Nobuki Kato Kengo Hayashi Sho Tozawa Dr. Yusuke Ogura Prof. Shigefumi Kuwahara Prof. Minoru Ueda 《ChemistryOpen》2020,9(10):1008-1017
An efficient and stereoselective syntheses of all the possible stereoisomers of coronafacic acid (CFA) has been developed. The stereochemistries of C3a and C7a were controlled in a diastereoselective Diels-Alder type cycloaddition using a chiral auxiliary. CFA and 6-epi-CFA were synthesized by hydrogenation of a common intermediate. During the synthesis of 6-epi-CFA, we established that its cis-fused configuration is important for the introduction of C4-C5 double bond by dehydration. This report is the first practical synthesis of both 6-epi-CFA, and its enantiomer. 相似文献
9.
A new approach to reduce the reverse current of Ge pin photodiodes on Si is presented, in which an i-Si layer is inserted between Ge and top Si layers to reduce the electric field in the Ge layer. Without post- growth annealing, the reverse current density is reduced to -10 mA/cm^2 at -1 V, i.e., over one order of magnitude lower than that of the reference photodiode without i-Si layer. However, the responsivity of the photodiodes is not severely compromised. This lowered-reverse-current is explained by band-pinning at the i-Si/i-Ge interface. Barrier lowering mechanism induced by E-field is also discussed. The presented "non-thermal" approach to reduce reverse current should accelerate electronics-photonics convergence by using Oe on the Si complementary metal oxide semiconductor (CMOS) platform. 相似文献
10.
Katsuyuki Ogura Kunio Sanada Kazumasa Takahashi Hirotada Iida 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1-2):83-87
Abstract An efficient preparation of a 3-methylthio-2-alkanone (1) has been realized by the reaction of a 3-alkyl-2,4-pentanedione (8) with one mol-equiv of S-methyl methanethiosulfonate (4) in the presence of excess EtONa in EtOH. Furthermore, treatment of 8 with 4 and K2CO3 in refluxing acetone, followed by addition of MeOH and heating the resulting mixture, gave 1 in a high yield. These methods were applied to synthesis of pseudoionone. 相似文献