Two inorganic–organic hybrid silver-polyoxometalates as reusable catalysts for one-pot synthesis of propargylamines via a three-component coupling reaction at room temperature,CrystEngComm

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Two inorganic–organic hybrid silver-polyoxometalates as reusable catalysts for one-pot synthesis of propargylamines via a three-component coupling reaction at room temperature
CrystEngComm ( IF 2.6 ) Pub Date : 2020-03-13 , DOI: 10.1039/d0ce00042f
Ming-Yu Dou _{1,

2,

3,

4,

5} , Xian-Qiang Huang _{6,

7,

8,

9,

10} , Guo-Yu Yang _{1,

2,

3,

4,

5}

Affiliation

By the combination of Ag-complexes and Keggin POMs, two novel inorganic–organic silver–polyoxometalates hybrids, [Ag₃L₂(DMSO)₂][PW₁₂O₄₀]·4DMSO (1) and [(Ag₂L₂)₂][SiW₁₂O₄₀]·10DMSO·2H₂O (2) (L = 4-(2-pyridyl)-6-(4-pyridyl)-2-aminopyrimidine), were synthesized and characterized. Interestingly, the silver atoms in compound 1 are three-coordinated with the AgNO model; however, the Ag atoms of compound 2 were surrounded by four N atoms of the organic ligands and displayed a distorted tetrahedral configuration. Importantly, compound 1 showed high catalytic activities for the three-component coupling reaction of alkynes and secondary amines along with formaldehyde, which resulted in a series of propargylamine derivatives in higher yields (up to 99%). Furthermore, the Ag–POM catalyst was easily recovered by filtration and reused for three cycles without a significant loss in catalytic activity. A tentative mechanism is also proposed for this transformation.

中文翻译：

两种无机-有机杂化银-多金属氧酸盐可重复使用的催化剂，用于在室温下通过三组分偶联反应一锅法合成炔丙胺

通过银络合物和Keggin POM的组合，形成了两种新型的无机-有机银-多金属氧酸盐杂化物[Ag ₃ L ₂（DMSO）₂ ] [PW ₁₂ O ₄₀ ]·4DMSO（1）和[（Ag ₂ L ₂）₂ ] [SiW ₁₂ O ₄₀ ]·10DMSO·2H ₂ O（2）（L ＝ 4-（2-吡啶基）-6-（4-吡啶基）-2-氨基嘧啶）被合成和表征。有趣的是，化合物1中的银原子与AgNO模型三配位；但是，化合物2的Ag原子被有机配体的四个N原子包围并显示出扭曲的四面体构型。重要的是，化合物1对炔烃和仲胺与甲醛的三组分偶联反应显示出高催化活性，从而以更高的收率（高达99％）产生了一系列炔丙基胺衍生物。此外，Ag-POM催化剂很容易通过过滤回收，并可以重复使用三个循环而不会显着降低催化活性。还为这种转换提出了一种尝试性机制。

更新日期：2020-04-24

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