Activity and selectivity control in reductive amination of butyraldehyde over noble metal catalysts

Activity and selectivity control in reductive amination of butyraldehyde over noble metal catalysts
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DOI:
10.1007/s10562-005-7431-4
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发表时间:
2005-10-01
期刊:
影响因子:
2.8
通讯作者:
Lercher, JA
Lercher, JA
中科院分区:
化学4区
文献类型:
--
作者:
Bödis, J;Lefferts, L;Lercher, JA

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探索了在碳负载贵金属催化剂(Ru、Rh、Pd 和 Pt)上控制丁醛与氨催化还原胺化的选择性和活性的方法。对反应网络的详细分析表明,席夫碱 N-[亚丁基]丁-1-胺是最重要的初始产物,只有在几乎所有丁醛都转化为 N-[亚丁基]丁-1-胺后,才在产物混合物中检测到胺。从该中间体中,良好的氢解催化剂(Ru、Rh)主要产生丁胺,而氢解活性较低的催化剂(Pd、Pt)则导致 N-[亚丁基]丁-1-胺氢化成大部分二丁胺。
Approaches to control selectivity and activity in the catalytic reductive amination of butyraldehyde with ammonia over carbon supported noble metal catalysts (Ru, Rh, Pd, and Pt) were explored. Detailed analysis of the reaction network shows that the Schiff base N-[butylidene]butan-1-amine is the most prominent initial product and, only after nearly all butyraldehyde had been converted to N-[butylidene]butan-1-amine, amines are detected in the product mixture. From this intermediate, good hydrogenolysis catalysts (Ru, Rh) produce mostly butylamine, while catalysts less active in hydrogenolysis (Pd, Pt) lead to the hydrogenation of N-[butylidene]butan-1-amine to mostly dibutylamine.