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Strategy to isolate ionic gold sites on silica surface: increasing their efficiency as catalyst for the formation of 1,3-diynes
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2020-02-01 , DOI: 10.1016/j.apcata.2020.117444
Cezar A. Didó , Felipe L. Coelho , Maurício B. Closs , Monique Deon , Flavio Horowitz , Fabiano Bernardi , Paulo H. Schneider , Edilson V. Benvenutti

A new strategy is presented to obtain an efficient heterogeneous gold catalyst constituted by isolated ionic gold sites, which is known to be effective in alkyne coupling reaction. The procedure is based on a significant difference between offered gold amount and available adsorbent sites on the support, ensuring the formation of very active isolated gold ion sites. In order to achieve this purpose, mesoporous silica xerogel was grafted with an ionic silsesquioxane containing charged ammonium quaternary group. The modified silica showed 0.25 mmol of cationic sites per gram of material and presented thermal stability up to 200 °C. This material was applied as support for immobilization of Au(III) ions as square planar AuCl4- complex. The gold amount offered was just 12% of the exchangeable capacity. The catalyst was efficiently applied in the cross coupling reactions, in which only 0.22 mol% was applied to obtain symmetric and non-symmetric 1,3-diynes.



中文翻译:

隔离二氧化硅表面离子金位的策略:提高其作为1,3-二炔形成催化剂的效率

提出了一种新的策略以获得由孤立的离子金位点构成的高效多相金催化剂,已知该催化剂对炔烃偶联反应有效。该程序基于提供的金量和载体上可用的吸附剂位点之间的显着差异,从而确保形成非常活跃的孤立金离子位点。为了实现该目的,将中孔二氧化硅干凝胶接枝了具有带电季铵盐基团的离子倍半硅氧烷。改性的二氧化硅在每克材料中显示0.25 mmol的阳离子位点,并在高达200°C的温度下具有热稳定性。该材料用作固定Au(III)离子的载体,作为方形平面AuCl 4-复杂。提供的黄金量仅为可交换量的12%。该催化剂被有效地用于交叉偶联反应中,其中仅施用0.22mol%以获得对称和不对称的1,3-二炔。

更新日期:2020-02-03
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