化工进展 ›› 2020, Vol. 39 ›› Issue (S1): 175-179.DOI: 10.16085/j.issn.1000-6613.2020-0172

• 工业催化 • 上一篇    下一篇

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

李石雄1,2(), 黄元浩1, 廖蓓玲2()   

  1. 1.梧州学院化学工程与资源再利用学院，广西 梧州 543002
    2.河池学院化学与生物工程学院，广西 河池 546300
  • 收稿日期:2020-02-06 出版日期:2020-05-20 发布日期:2020-06-29
  • 通讯作者: 廖蓓玲
  • 作者简介:李石雄（1985—），男，博士研究生，研究方向为功能材料和水资源回用技术。E-mail：lsx1324@163.com。
  • 基金资助:
    广西科技基地和人才专项(AD19245031);广西自然科学基金(2019GXNSFBA245063);梧州学院开放实验室创新性实验(2019005);河池市科技项目(2019025)

C—C bond cleavage by zinc(Ⅱ) complex and in-situ synthesis of2-methyl-4(3H)-quinazolinone

Shixiong LI1,2(), Yuanhao HUANG1, Beiling LIAO2()   

  1. 1.School of Chemical Engineering and Resource Recycling, Wuzhou University, Wuzhou 543002, Guangxi, China
    2.School of Chemistry and Biological Engineering, Hechi University, Hechi 546300, Guangxi, China
  • Received:2020-02-06 Online:2020-05-20 Published:2020-06-29
  • Contact: Beiling LIAO

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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CC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CC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。

关键词: 配位化合物, 合成, 结构, 催化

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(3H)-quinazolinone is synthesized in-situ by [Zn(L)2·(H2O)2·(NO3)2] (where L=4(3H)-quinazolinone) complex to catalyzes the CC bond cleavage of acetonitrile under 130℃. The structures of 2-methyl-4(3H)-quinazolinone and [Zn(L)2·(H2O)2·(NO3)2] are characterized by IR, elemental analysis, and X-ray single crystal diffraction. The results show that [Zn(L)2·(H2O)2·(NO3)2] and 2-methyl-4 (3H) -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 (3H) -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 (3H)-quinazolone. It was found that [Zn(L)2·(H2O)2·(NO3)2] catalyzed the CC 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.

Key words: complex, synthesis, structure, catalysis

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