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Tsvetkov N. P. Vakhmistrov V. E. Koldobsky A. B. Korlyukov A. A. Kalinin V. N. 《Russian Chemical Bulletin》2002,51(2):326-331
Unusual cascade cycloaddition reactions with dimethylhydrazones of -trimethylsilyloxyalkylacroleins acting as azadienes were found. Depending on the nature of the dienophile, the reactions give either fused heterocyclic compounds (when two consecutive Diels—Alder reactions take place) or azabicyclic compounds, resulting from the [2+4]- and [2+3]-cycloaddition cascade. 相似文献
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Brønsted acid-catalyzed inverse-electron demand (IED) aza-Diels-Alder reactions between 2-aza-dienes and ethylene were studied using quantum chemical calculations. The computed activation energy systematically decreases as the basic sites of the diene progressively become protonated. Our activation strain and Kohn-Sham molecular orbital analyses traced the origin of this enhanced reactivity to i) “Pauli-lowering catalysis” for mono-protonated 2-aza-dienes due to the induction of an asynchronous, but still concerted, reaction pathway that reduces the Pauli repulsion between the reactants; and ii) “LUMO-lowering catalysis” for multi-protonated 2-aza-dienes due to their highly stabilized LUMO(s) and more concerted synchronous reaction path that facilitates more efficient orbital overlaps in IED interactions. In all, we illustrate how the novel concept of “Pauli-lowering catalysis” can be overruled by the traditional concept of “LUMO-lowering catalysis” when the degree of LUMO stabilization is extreme as in the case of multi-protonated 2-aza-dienes. 相似文献
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《Tetrahedron》2003,59(15):2617-2623
Simple and functionalized N-phosphorylalkyl imines and N-phosphorylalkyl-N′-phenyl-carbodiimides are obtained by aza-Wittig reaction of phosphazenes derived from aminophosphonates with carbonyl compounds and phenyl isocyanate. The reaction with dimethylformamide diethyl acetal (DMF-DEA) of these functionalized imines leads to the synthesis of 4-amino-3-phosphoryl-2-azadienes. N-Phosphorylmethyl imine derived from benzaldehyde can be used for the preparation of substituted pyrrole-phosphonates, while acid treatment of 4-dimethylamino-3-diethylphosphoryl-1-phenyl-2-azadiene gives diethyl 5-diethylphosphorylpyrazin-2-ylphosphonate. 相似文献
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Sodium Salts of Anionic Chiral Cobalt(III) Complexes as Catalysts of the Enantioselective Povarov Reaction 下载免费PDF全文
Dr. Jie Yu Hua‐Jie Jiang Ya Zhou Prof. Dr. Shi‐Wei Luo Prof. Dr. Liu‐Zhu Gong 《Angewandte Chemie (International ed. in English)》2015,54(38):11209-11213
The sodium salts of anionic chiral cobalt(III) complexes (CCC?Na+) have been found to be efficient catalysts of the asymmetric Povarov reaction of easily accessible dienophiles, such as 2,3‐dihydrofuran, ethyl vinyl ether, and an N‐protected 2,3‐dihydropyrrole, with 2‐azadienes. Ring‐fused tetrahydroquinolines with up to three contiguous stereogenic centers were thus obtained in high yields, excellent diastereoselectivities (endo/exo up to >20:1), and high enantioselectivities (up to 95:5 e.r.). 相似文献
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Vahmistrov V. E. Tsvetkov N. P. Koldobsky A. B. Vorontsov E. V. Kalinin V. N. 《Russian Chemical Bulletin》2004,53(1):233-235
A series of new -substituted acrolein dimethylhydrazones containing an acetal group were synthesized. These hydrazones react with acrylonitrile or methyl acrylate according to the Diels—Alder reaction pattern to give substituted tetrahydropyridines. An unusual [2+4]- and [2+3]-cycloaddition cascade reaction involving -diethoxymethylacrolein dimethylhydrazone was discovered. 相似文献
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Brønsted acid‐catalyzed inverse‐electron demand (IED) aza‐Diels‐Alder reactions between 2‐aza‐dienes and ethylene were studied using quantum chemical calculations. The computed activation energy systematically decreases as the basic sites of the diene progressively become protonated. Our activation strain and Kohn‐Sham molecular orbital analyses traced the origin of this enhanced reactivity to i) “Pauli‐lowering catalysis” for mono‐protonated 2‐aza‐dienes due to the induction of an asynchronous, but still concerted, reaction pathway that reduces the Pauli repulsion between the reactants; and ii) “LUMO‐lowering catalysis” for multi‐protonated 2‐aza‐dienes due to their highly stabilized LUMO(s) and more concerted synchronous reaction path that facilitates more efficient orbital overlaps in IED interactions. In all, we illustrate how the novel concept of “Pauli‐lowering catalysis” can be overruled by the traditional concept of “LUMO‐lowering catalysis” when the degree of LUMO stabilization is extreme as in the case of multi‐protonated 2‐aza‐dienes. 相似文献
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Wen-Dao Chu Chun-Mei Wang Jie Zhan Ya-Li Zeng Yong Liu Bo Chen Kaiming Zhang Cheng-Yu He Quan-Zhong Liu 《European journal of organic chemistry》2023,26(16):e202300210
Copper-catalyzed 1,4-addition of a silicon nucleophile to azadienes is reported. This method facilely provided a wide variety of dibenzylic silane derivatives in good to excellent yields. The important practical features are the use of a cheap catalytic system, mild reaction conditions, and broad substrate scope. 相似文献
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