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Direct competitions of intramolecular C - H insertions into benzylic C - H and 4-nitroor 4-methoxy substituted benzylic C - H of methyl 2-diazo-3-oxo-6-(4-substituted phenyl)-4-(2-phenylethyl)hexanoate 44a and 44b catalyzed by Rh-mediated carbenoid were alsoinvestigated, and the relative reactivities obtained by compound 44a or 44b were comparableto those obtained by indirect method.

此外,还研究了Rh催化分解下,对位硝基取代或甲氧基取代的4-(2-苯基乙基)-6-(4-取代苯基)-2-重氮基-3-氧代己酸甲酯44a、44b苯甲位C-H插入反应的相对速率,与化合物47a和47f得到的结果比较,数据平行。

Therelative rates of the Rh-mediated carbenoid insertion into the benzylic C - H bonds of aseries of para-substituted phenyl substrates: methyl 2-diazo-3-oxo-6-(4-substituted phenyl)-4-propylhexanoate 47a - g, have been measured by an indirect intramolecular competitionmethod under the condition in which the possible steric and conformational effects have beenminimized.

为了将立体因素和构象因素最大程度减小,以便较为准确地评价电子效应对该反应的影响,设计并合成了不同对位取代基的化合物4-丙基-6-(4-取代苯基)-2-重氮基-3-氧代己酸甲酯47a-g,并研究了它们在不同Rh催化剂作用下的分子内C-H插入反应。

The mixed trimeric compounds containing one ferrocene unit, N,N'-bis(2-hydroxy-5-substituted benzylidene)ferrocenylmethylenediamine, have been synthesized directly through the reaction between 1 mol of ferrocenecarboxaldehyde and 2 mol of 5-substituted salicylaldehyde.

通过甲酰基二茂铁与取代水杨醛和氨反应,直接合成了含一个二茂铁的混合三聚产物, N,N'-二[2-羟基-5-取代苄烯]二茂铁甲二胺。

Based on above analysis, a series of novel pentadiynes substituted with pyrimidinyl group were synthesised, and the reaction between them and C60 was applied to synthesize fullerene derivatives of diacetylene substituted by pyrimidine groups.

根据以上设想设计合成了一系列嘧啶基取代戊二炔衍生物,使之与C60反应,合成了嘧啶基取代炔类C60衍生物。

The chapter two was focused on the samarium diiodide promoted organic reactions and their applications in organic synthesis, firstly, a new synthesis of highly substituted cyclopentadienes from a,β-alkynone promoted by samarium diiodide was investigated and the highly substituted cyclopentadienes were prepared in moderate to good yields under mild conditions. Secondly, the Michael addition and Michael-aldol tandem reaction of diorganyl diselenides or diorganyl disulfides with α,β-alkynones mediated by samarium diiodide were studied and a series of alkenylsulfides and alkenylselenides were prepared in good yields. Then the highly regioselecfive nucleophilic addition of the allylsamarium bromide to α,β-alkynones were explored. We found that the allylsamarium bromide reacts with α,β-alkynones to afford regiospecificly 1. 2-nucleophilic addition products in good yields under mild condition. At last we studied the coupling reaction of aryl halides promoted by NiCl〓/PPh〓/Sm〓.

第二章 研究了二碘化钐、金属钐促进的有机反应:1、二碘化钐促进下α,β-炔基酮的偶联环化反应,提供了一种制备多取代环戊二烯的新方法;2、二碘化钐促进下的二硫醚、二硒醚与α,β-炔基酮的Michael加成反应,为高产率地制备多取代的烯基硫或烯基硒化合物提供了方便可靠的新方法;3、二碘化钐促进下的二硫醚、二硒醚与α,β-炔基酮和醛、酮的Michael—aldol串联反应,提供了一种一锅法高产率地制备多取代的含硫的烯丙基醇或含硒的烯丙基醇类化合物的方便可靠的原子经济性的新方法;4、烯丙基溴化钐与α,β-炔基酮的高度区域选择性的1,2-亲核加成反应;5、NiCl〓/PPh〓/Sm〓促进的卤代芳烃的偶联反应-一种从各种卤代芳烃制备联苯类化合物的有效方法。

This dissertation is mainly focused on the reactivity of methylenecyclopropanes and comprises six parts. 1 The reactions of methylenecyclopropanes with phenylsulfenyl chloride, phenylselenyl chloride and diphenyl diselenide; 2 The coupling reactions of the ring-opening products derivated from methylenecyclopropanes; 3 The palladium-catalyzed ring-enlargement of mono-aryl group substituted methylenecyclopropanes to cyclobutenes. 4 The gold-catalyzed domino ring-opening and ring-closing hydroamination of methylenecyclopropanes with sulfonamides; 5 The Lewis acid-catalyzed reactions of mono-aryl group substituted methylenecyclopropanes with diethyl ketomalonate in the presence of water; 6 The iodobenzene diacetate mediated novel 1,3-dipolar cycloaddition of methylenecyclopropanes, vinylidenecyclopropanes, and methylenecyclobutane with phthalhydrazine.

本论文主要研究了亚甲基环丙烷类化合物的一些化学反应性能,共由以下六部分组成:1、亚甲基环丙烷类化合物与苯硫氯、苯硒氯及二苯基二硒的反应;2、亚甲基环丙烷类化合物开环产物的偶联反应;3、单芳基取代的亚甲基环丙烷类化合物在钯催化剂作用下的扩环反应;4、金化合物催化磺酰胺对亚甲基环丙烷类化合物的串联开环关环氨氢化反应;5、路易斯酸催化亚甲基环丙烷类化合物与丙酮二羧酸二乙酯在有水存在下的反应;6、醋酸碘苯促进的亚甲基环丙烷类化合物、亚乙烯基环丙烷类化合物及亚甲基环丁烷类化合物与邻苯二甲酰肼的新型1,3-偶极环加成反应。

Totally 17 new type of fulvene ligands have been synthesized by the reaction of substituted-benzoyl chloride with Cp and substituted Cp anions. All the new compounds are fully characterized by infrared spectroscopy,!

我们利用含芳香取代基的环戊二烯丛负离子与含-CN、-I、-CO_2CH_3等配位有机基团的芳酰氯反应成功地合成了17个既含芳香基团又含杂原子配位基团的刚性共轭富烯类配体。

1Five novel E-(4-β-D-allopyranosyloxyphenyl)-1-(4-substituted phenyl) propenone derivatives were designed and synthesized by the Claisen-Schimidt reaction with 4-substituted hypnone.

1与4-取代苯乙酮进行Claisen-Schimidt缩合,合成了五个未见文献报道的E-4-β-D-吡喃阿洛糖苷-苯乙烯基-4-取代苯酮衍生物。

A mild and convenient method for the synthesis of 4(3)-substituted 3(4)-nitro-1H-pyrroles and 3-substituted 4-methyl-2-tosyl-1H-pyrroles from nitroolefins and tosylmethyl isocyanide in ionic liquid 1-butyl-3- methylimidazolium bromide was developed.

本文以离子液体-溴化1-丁基-3-甲基咪唑为溶剂,采用对甲苯磺酰基甲基异腈与硝基烯反应生成4(3)-取代-3(4)-硝基-1-氢吡咯或3-取代-4-甲基-2-对甲苯磺酰基-1-氢吡咯。

Furthermore, the one-dimensional complexes 26 and 28 with strongπ-πpacking interactions are prepared from DMF solvent, which indicates that the traditional solvent volatilizing method could bring low-dimensional complex.4. By measuring the enthalpy changes of the liquid phase formation reaction for complexes a~e, and calculating the electronic densities of five 5-substituted derivation of isophthalic acid, we can make a conclusion that 5-substituted group changing of the ligand has a little influence on oxygen atoms of carboxyl groups.5. Fluorescence experiments of these complexes indicated that they could be used for luminescence materials in future.6. Using packing saturation rule we calculated and analyzed these series of complexes, and the results showed that the changes of complexes with changes of ligands could be explained from the rule.

在DMF溶剂中得到了具有强π-π堆积作用力的一维配位聚合物[Ln(5-NO_2-bdc)(NO_3)]Ln=Pr(26和Ho(28),表明传统的溶剂挥发合成条件可以得到低维的配合物。4、通过配合物a~e的液相生成反应焓的测定,以及配体阳离子的电子密度计算,进一步佐证了间苯二甲酸的5位取代基变化对配体的羧基氧原子配位能力影响不大的结论。5、荧光特性表明此类配合物可以用于发光材料。6、利用堆积饱和规律对所得系列的配合物的进行计算和分析,发现随着配体的变化,配合物的变化可以从堆积饱和规律出发进行解释。

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