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Zn(Ⅱ)配合物催化C—C键裂解和原位合成2-甲基-4(3H)-喹唑酮
C—C bond cleavage by zinc(Ⅱ) complex and in-situ synthesis of 2-methyl-4(3H)-quinazolinone
【摘要】 在配合物的水热合成过程中往往可以发现新的化学反应和催化机理。本文通过[Zn（L）2·（H2O）2·（NO3）2]（L=4（3H）-喹唑酮）配合物在130℃催化乙腈分子中的C—C键断裂,原位合成化合物2-甲基-4（3H）-喹唑酮。利用红外、元素分析和X射线单晶衍射表征分析2-甲基-4（3H）-喹唑酮和[Zn（L）2·（H2O）2·（NO3）2]的结构,结果表明[Zn（L）2·（H2O）2·（NO3）2]和2-甲基-4（3H）-喹唑酮属于三斜晶系,P-1空间群。三组温度控制实验表明,温度对2-甲基-4（3H）-喹唑啉酮的形成有着重要的影响,并且温度高于130℃有利于该催化反应的进行。采取电喷雾质谱表征2-甲基-4（3H）-喹唑酮的形成机理发现,[Zn（L）2·（H2O）2·（NO3）2]催化乙腈分子中的C—C键断裂,生成（CN）2和·CH3。·CH3有选择性地引入到4（3H）-喹唑酮中的C原子和N原子之间。本文对原位引入—CH3有着指导作用。
【Abstract】 New chemical reactions and catalytic mechanisms can be found in the hydrothermal synthesis of complexes or compounds.In this paper,the compound of 2-methyl-4（3 H）-quinazolinone is synthesized in-situ by [Zn（L）2·（H2 O）2·（NO3）2]（where L=4（3 H）-quinazolinone） complex to catalyzes the C—C bond cleavage of acetonitrile under 130℃.The structures of 2-methyl-4（3 H）-quinazolinone and [Zn（L）2·（H2 O）2·（NO3）2]are characterized by IR,elemental analysis,and X-ray single crystal diffraction.The results show that[Zn（L）2·（H2 O）2·（NO3）2] and 2-methyl-4（3 H）-quinazolone belong to the triclinic system and P-1 space group.Three sets of temperature control experiments show that the temperature has an important effect on the formation of 2-methyl-4（3 H）-quinazolinone,and that the temperature is higher than 130℃ is conducive to the catalytic reaction.The electrospray mass spectrometry（ESI-MS） was used to characterize the formation mechanism of 2-methyl-4（3 H）-quinazolone.It was found that [Zn（L）2·（H2 O）2·（NO3）2] catalyzed the C—C cleavage in the acetonitrile molecule to produce（CN）2 and ·CH3.The ·CH3 is selectively introduced between the C and N atoms in 4（3H）-quinazolone.This paper has a guiding effect on the in-situ introduction of —CH3.
- 【文献出处】 化工进展 ,Chemical Industry and Engineering Progress , 编辑部邮箱 ,2020年S1期
- 【分类号】O641.4;O626
- 【下载频次】49