Asymmetric Conjugate Addition of Unmodified Cyclic Ketones to Nitroolefins Using Aminophosphonate as the Organocatalyst

本文设计合成了光学纯吡咯烷基磷酸酯,并成功地应用于酮类底物与b-硝基芳基乙烯衍生物的不对称催化Michael加成反应中。在20 mol %催化剂用量下,以10 mol %三氟乙酸作为添加物,无溶剂条件下,0 oC反应7-24小时,Michael加成产物的收率最高达96%,非对映选择性最高可达97:3,ee值最高可达90%。     

L-脯氨酸催化不对称有机反应的研究进展

综述了L-脯氨酸作为有机小分子催化剂在若干不对称有机反应(如Aldol反应,Mannich反应,共轭加成等)中的研究进展.参考文献33篇.     

过渡金属电解水催化剂的非金属掺杂研究进展

过渡金属基材料成本相对较低,催化性能较为优异,是在全水分解领域最有希望替代贵金属基电催化剂的候选材料之一,但有限的活性位点、相对较差的电导率等因素限制了其广泛应用。非金属元素掺杂能够调节主体材料电子结构,优化吸附能,从而对过渡金属基电催化剂的活性与稳定性产生积极影响,缩减其与贵金属材料性能差距。本文总结了近年来非金属元素改性在过渡金属基电催化材料中的相关研究,系统综述了非金属元素掺杂的方法和不同非金属元素的掺杂效果,从物理化学性质的改变和电子结构的变化多角度分析了非金属元素改性对过渡金属基材料的影响,最后对非金属元素掺杂过渡金属基电催化剂的未来发展方向作出了展望。     

Organocatalyzed Double C(sp3)−H Alkylation of Cyclic N-Sulfonyl Ketimines with 3-Chloropropiophenones: Selective Access to 2,3,6-Trisubstituted Pyridines

An efficient sequential one-pot, two-step pseudo-four-component reaction between 3/4-methyl N-sulfonyl ketimines with 3-chloropropiophenones triggered by DIPEA/NaHCO₃ as a cooperative base and subsequent aza-cyclization using NH₄OAc is reported. This transition-metal-oxidant-free technique concocts new C−C/C=C/C=N−C bonds selectively, guaranteeing acceptable yields of 2,3,6-trisubstituted pyridines possessing ortho-hydroxyaryl/benzenesulfonamide and propiophenone moieties at C2 and C3 positions, respectively. Interestingly, while replacing methyl-substituents with straight alkyl chains of N-sulfonyl ketimines, only a monoalkylation reaction happened with in situ-generated vinyl ketones to deliver promising yields of 3-picoline derivatives. Moreover, the synthetic transmutation of prepared pyridine derivative led to several important classes of pyridocoumarin, 5H-chromenopyridine, and di(pyridin-3-yl) methane derivatives.     

Organocatalytic Synthesis of Chiral Halogenated Compounds

This account summarizes our recent efforts in the enantioselective organocatalytic synthesis of chiral halogenated compounds. The enantioselective α-halogenation of aldehydes, decarboxylative chlorination of β-keto acids, and enantioselective C−C bond formation at the trifluoromethylated prochiral carbon to yield the corresponding organohalides with chlorinated, fluorinated, or trifluoromethylated chiral stereogenic centers are discussed. We applied common organocatalysts, such as Jørgensen-Hayashi catalyst and cinchona alkaloid-derivatived catalyst, and developed novel chiral amine catalysts for these reactions. This account also discusses stereospecific derivatizations of the resulting chiral halogenated compounds via nucleophilic substitution. Thus, we synthesized many novel chiral compounds that have not been reported, even as racemates.