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A spatially orthogonal hierarchically porous acid–base catalyst for cascade and antagonistic reactions
Nature Catalysis ( IF 42.8 ) Pub Date : 2020-10-26 , DOI: 10.1038/s41929-020-00526-5
Mark A. Isaacs , Christopher M. A. Parlett , Neil Robinson , Lee J. Durndell , Jinesh C. Manayil , Simon K. Beaumont , Shan Jiang , Nicole S. Hondow , Alexander C. Lamb , Deshetti Jampaiah , Michael L. Johns , Karen Wilson , Adam F. Lee

Complex organic molecules are of great importance to research and industrial chemistry and typically synthesized from smaller building blocks by multistep reactions. The ability to perform multiple (distinct) transformations in a single reactor would greatly reduce the number of manipulations required for chemical manufacturing, and hence the development of multifunctional catalysts for such one-pot reactions is highly desirable. Here we report the synthesis of a hierarchically porous framework, in which the macropores are selectively functionalized with a sulfated zirconia solid acid coating, while the mesopores are selectively functionalized with MgO solid base nanoparticles. Active site compartmentalization and substrate channelling protects base-catalysed triacylglyceride transesterification from poisoning by free fatty acid impurities (even at 50 mol%), and promotes the efficient two-step cascade deacetalization-Knoevenagel condensation of dimethyl acetals to cyanoates.



中文翻译:

空间正交的分层多孔酸碱催化剂,用于级联反应和拮抗反应

复杂的有机分子对研究和工业化学非常重要,通常通过多步反应由较小的结构单元合成。在单个反应器中进行多次(不同)转化的能力将大大减少化学生产所需的操作数量,因此,非常需要开发用于这种一锅法反应的多功能催化剂。在这里我们报告了分层多孔框架的合成,其中大孔被硫酸化的氧化锆固体酸涂层选择性地功能化,而中孔被MgO固体基础纳米粒子选择性地功能化。

更新日期:2020-10-28
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