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首页> 外文期刊>Chemistry: A European journal >Catalytic Hydrogen Production by Ruthenium Complexes from the Conversion of Primary Amines to Nitriles: Potential Application as a Liquid Organic Hydrogen Carrier
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Catalytic Hydrogen Production by Ruthenium Complexes from the Conversion of Primary Amines to Nitriles: Potential Application as a Liquid Organic Hydrogen Carrier

机译：从伯胺向腈转化为钌配合物的催化氢生产：作为液体有机氢载体的潜在应用

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摘要

The potential application of the primary amineitrile pair as a liquid organic hydrogen carrier (LOHC) has been evaluated. Ruthenium complexes of formula [(p-cym)Ru(NHC)Cl-2] (NHC=N-heterocyclic carbene) catalyze the acceptorless dehydrogenation of primary amines to nitriles with the formation of molecular hydrogen. Notably, the reaction proceeds without any external additive, under air, and under mild reaction conditions. The catalytic properties of a ruthenium complex supported on the surface of graphene have been explored for reutilization purposes. The ruthenium-supported catalyst is active for at least 10 runs without any apparent loss of activity. The results obtained in terms of catalytic activity, stability, and recyclability are encouraging for the potential application of the amineitrile pair as a LOHC. The main challenge in the dehydrogenation of benzylamines is the selectivity control, such as avoiding the formation of imine byproducts due to transamination reactions. Herein, selectivity has been achieved by using long-chain primary amines such as dodecylamine. Mechanistic studies have been performed to rationalize the key factors involved in the activity and selectivity of the catalysts in the dehydrogenation of amines. The experimental results suggest that the catalyst resting state contains a coordinated amine.
机译：已经评估了伯胺/腈对作为液态有机氢载体（LOHC）的潜在应用。式[（p-cym）Ru（NHC）Cl-2]（NHC = N-杂环卡宾）的钌络合物催化伯胺的无受体脱氢为腈，并形成分子氢。值得注意的是，该反应在没有任何外部添加剂的情况下在空气和温和的反应条件下进行。为了再利用，已经研究了负载在石墨烯表面上的钌配合物的催化性能。钌负载催化剂具有至少10次运行的活性，而活性没有明显降低。在催化活性，稳定性和可循环性方面获得的结果对于胺/腈对作为LOHC的潜在应用是令人鼓舞的。苄胺脱氢的主要挑战是选择性控制，例如避免由于氨基转移反应而形成亚胺副产物。在此，通过使用长链伯胺如十二烷基胺实现了选择性。已经进行了机理研究以使胺脱氢中涉及催化剂活性和选择性的关键因素合理化。实验结果表明，催化剂的静止状态含有配位胺。

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