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MOF-derived cobalt nanoparticles catalyze a general synthesis of amines
Science ( IF 56.9 ) Pub Date : 2017-09-21 , DOI: 10.1126/science.aan6245
Rajenahally V. Jagadeesh 1 , Kathiravan Murugesan 1 , Ahmad S. Alshammari 2 , Helfried Neumann 1 , Marga-Martina Pohl 1 , Jörg Radnik 1 , Matthias Beller 1
Affiliation  

A MOF sets the stage to make amines Reductive amination is a common method that chemists use to make carbon-nitrogen bonds. The reaction, which often requires precious metal catalysts, couples ammonia or other amines with carbonyl compounds and then with hydrogen. Jagadeesh et al. report a class of nonprecious cobalt nanoparticles that catalyze this reaction across a very broad range of substrates, including complex molecules of pharmaceutical interest (see the Perspective by Chen and Xu). The cobalt was first embedded in a metal-organic framework (MOF), which, upon heating, transformed into a graphitic shell. The catalyst could be conveniently separated from products and recycled up to six times. Science, this issue p. 326; see also p. 304 Cobalt nanoparticles prepared from a metal-organic framework precursor catalyze a very broad range of reductive aminations. The development of base metal catalysts for the synthesis of pharmaceutically relevant compounds remains an important goal of chemical research. Here, we report that cobalt nanoparticles encapsulated by a graphitic shell are broadly effective reductive amination catalysts. Their convenient and practical preparation entailed template assembly of cobalt-diamine-dicarboxylic acid metal organic frameworks on carbon and subsequent pyrolysis under inert atmosphere. The resulting stable and reusable catalysts were active for synthesis of primary, secondary, tertiary, and N-methylamines (more than 140 examples). The reaction couples easily accessible carbonyl compounds (aldehydes and ketones) with ammonia, amines, or nitro compounds, and molecular hydrogen under industrially viable and scalable conditions, offering cost-effective access to numerous amines, amino acid derivatives, and more complex drug targets.

中文翻译:

MOF 衍生的钴纳米粒子催化胺的一般合成

MOF 为制造胺奠定了基础 还原胺化是化学家用来制造碳氮键的常用方法。该反应通常需要贵金属催化剂,将氨或其他胺与羰基化合物偶联,然后与氢气偶联。贾加迪什等人。报告了一类非贵重的钴纳米粒子,可在非常广泛的底物上催化这种反应,包括具有药用价值的复杂分子(参见 Chen 和 Xu 的观点)。钴首先嵌入金属有机框架 (MOF) 中,加热后转变为石墨壳。催化剂可以方便地从产品中分离出来,最多可循环使用六次。科学,这个问题 p。326; 另见第。304 由金属-有机骨架前体制备的钴纳米颗粒可催化非常广泛的还原胺化反应。用于合成药物相关化合物的贱金属催化剂的开发仍然是化学研究的一个重要目标。在这里,我们报告说,由石墨壳包裹的钴纳米颗粒是广泛有效的还原胺化催化剂。它们方便实用的制备需要在碳上模板组装钴-二胺-二羧酸金属有机骨架,然后在惰性气氛下热解。所得稳定且可重复使用的催化剂对于合成伯胺、仲胺、叔胺和 N-甲胺(超过 140 个例子)具有活性。该反应将容易获得的羰基化合物(醛和酮)与氨、胺、
更新日期:2017-09-21
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