铱
催化作用
反应性(心理学)
烷基化
磷化氢
选择性
组合化学
金属有机骨架
配体(生物化学)
化学
金属
材料科学
有机化学
吸附
光化学
医学
生物化学
替代医学
受体
病理
作者
Wenmiao Chen,Muhammad Sohail,Veeranna Yempally,Yihao Yang,Ashfaq A. Bengali,Hong‐Cai Zhou,Sherzod T. Madrahimov
标识
DOI:10.1021/acsami.4c02143
摘要
Further development in the area of medicinal chemistry requires facile and atom-economical C-N bond formation from readily accessible precursors using recyclable and reusable catalysts with low process toxicity. In this work, direct N-alkylation of amines with alcohols is performed with a series of Ir-phosphine-functionalized metal-organic framework (MOF) heterogeneous catalysts. The grafted monophosphine-Ir complexes were studied comprehensively to illustrate the ligand-dependent reactivity. The afforded MOF catalysts exhibited high reactivity and selectivity toward N-alkylamine product formation, especially UiO-66-PPh2-Ir, which showed 90% conversion after recycling with no catalyst residue remaining in the product after the reaction. Furthermore, analyses of the active catalyst, mechanistic studies, control experiments, and H2 adsorption tests are consistent with the conclusion that immobilization of the iridium complex on the MOF support enables the formation of the iridium-monophosphine complex and enhances its stability during the reaction. To illustrate the potential of the catalyst for application in medicinal chemistry, two pharmaceutical precursors were synthesized with up to 99% conversion and selectivity.
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