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1.
Gonzalo Blay 《Tetrahedron》2004,60(1):165-170
The reaction of the lithium enolate of the (S,S)-cis-1,3-dioxolan-4-one derived from optically active (S)-mandelic acid and pivalaldehyde with several aromatic nitroalkenes in the presence of HMPA proceeds readily to give the corresponding Michael adducts in good yields and diastereoselectivities. Reduction of the nitro group with Zn/HCl/EtOH/H2O with concomitant intramolecular aminolysis of the acetal moiety leads directly to enantiomerically pure α-hydroxy-α,β-diaryl-γ-lactams.  相似文献   
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张崃  肖检  王雅雯  彭羽 《化学学报》2022,80(8):1152-1164
二氢苯并呋喃结构单元广泛存在于具有良好生物活性和药用价值的天然产物之中, 因而引起了有机合成化学家和药物化学家们的关注. 针对该结构单元所包含的C2和C3邻二立体中心的对映选择性构建, 也是目前有机合成方法学研究的挑战性问题之一. 在众多解决方案中, 以苯酚(醌)与烯烃为底物, 具体采用催化不对称和手性辅剂诱导的[3+2]环化两种方式, 可以构建具有光学活性的二氢苯并呋喃结构单元. 本综述将不同类型的手性催化剂和手性辅剂进行分类梳理, 介绍了近年来不对称[3+2]环化反应的发展, 并重点剖析其中涉及的立体选择性控制. 同时, 简要介绍了该关键方法在二氢苯并呋喃天然产物合成中的应用. 为了启发更加高效和普适性的新催化体系出现, 最后总结和展望了不对称[3+2]环化反应的发展趋势.  相似文献   
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Allylic pinacol boronic esters are stable toward 1,3‐borotropic rearrangement. We developed a PdII‐mediated isomerization process that gives di‐ or trisubstituted allylic boronic esters with high E selectivity. The combination of this method with lithiation–borylation enables the synthesis of carbon chains that bear 1,5‐stereogenic centers. The utility of this method has been demonstrated in a formal synthesis of (+)‐jasplakinolide.  相似文献   
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Chiral propargyl amines are valuable synthetic intermediates for the preparation of biologically active compounds and functionalized amines. Catalytic methods to access propargyl amines containing vicinal stereocenters with high diastereoselectivity are particularly rare. We report an unprecedented strategy for the synthesis of enantioenriched propargyl amines with two stereogenic centres. An iridium complex, ligated by a phosphoramidite ligand, catalyzes the hydroalkynylation of β,β‐disubstituted enamides to afford propargyl amides in a highly regio‐, diastereo‐, and enantioselective fashion. Stereodivergent synthesis of all four possible stereoisomers was achieved using this strategy.  相似文献   
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In nanoscience and nanotechnology, much attention has been given to the dual problem of designing nanocomponents with novel physical properties and how such nanocomponents can be fabricated. Receiving less attention has been the question of the nanocomponent's reliability; how does a nanocomponent fail and how long does a nanocomponent survive under typical operating conditions? High reliability is necessary to guarantee the advancement and utilization of nanocomponents due to the fact that they account for a high proportion of costs of newly designed nanosystems as well as multiscale systems. A nanocomponent is a component that is made of atoms, and its reliability is determined by these atoms. There are situations where it is hard or impossible to extract information from a nanocomponent about its relationship to its atoms. In this article, we assess the nanocomponent's reliability by using its physical properties. Specifically, it is known that nanocrack growth involves considerable statistical variability and such variability should be accounted for assessing growth. In this paper, we first provide a stochastic nanocrack growth model and then evaluate the reliability of a nanocomponent based on this model. Various properties of this model are obtained. We also evaluate the reliability of a nanocomponent under different assumptions on our proposed growth model. This paper is a modification of the extensive literature on modeling fatigue cracks in materials on a larger scale, applied to nanoscale where growth is not a function of cumulative stress on the component but related to the time to first exceedance of a threshold. Copyright © 2013 John Wiley & Sons, Ltd.  相似文献   
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The first total synthesis of (±)-heptemerone G, a diterpenoid metabolite of a submerged culture Coprinus heptemerus, and a new approach to an advanced intermediate for a synthesis of guanacastepene A are reported.  相似文献   
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Bis‐heteroaryl or bis‐aryl stereocenters were formed by an organocatalytic enantioselective conjugate addition using the respective trifluoroborate salts as nucleophiles. Control studies suggested that fluoride dissociation is necessary in the anhydrous conditions. This strategy is applicable to the synthesis of discoipyrrole D, an inhibitor of BR5 fibroblast migration.  相似文献   
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