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用于储氢的多相镍催化N-杂环的可逆、无受体脱氢反应。

Heterogeneous nickel-catalysed reversible, acceptorless dehydrogenation of N-heterocycles for hydrogen storage.

作者信息

Ryabchuk Pavel, Agapova Anastasiya, Kreyenschulte Carsten, Lund Henrik, Junge Henrik, Junge Kathrin, Beller Matthias

机构信息

Leibniz-Institut für Katalyse e. V. an der Universität Rostock, Albert-Einstein-Straße 29a, 18059 Rostock, Germany.

出版信息

Chem Commun (Camb). 2019 Apr 23;55(34):4969-4972. doi: 10.1039/c9cc00918c.

Abstract

Nickel-based nanocatalysts were used in acceptorless, reversible dehydrogenation and hydrogenation reactions of N-heterocycles. Both processes were realized in the same solvent using a single catalyst, without isolation of products and workup, which makes it attractive for hydrogen storage purposes. This concept has been demonstrated in a continuous hydrogenation/dehydrogenation sequence of quinaldine with negligible loss in activity of the nickel catalyst after three hydrogen storage cycles. The scope of acceptorless dehydrogenation has been explored and control experiments suggest that hydrogen liberation is initiated via amine dehydrogenation and supports the direct alkane dehydrogenation from the partially oxidized N-heterocycles.

摘要

镍基纳米催化剂用于N-杂环的无受体可逆脱氢和氢化反应。这两个过程在同一溶剂中使用单一催化剂即可实现,无需分离产物和后处理,这使其在储氢方面具有吸引力。喹哪啶的连续氢化/脱氢序列已证明了这一概念,在三个储氢循环后,镍催化剂的活性损失可忽略不计。已探索了无受体脱氢的范围,对照实验表明,氢的释放是通过胺脱氢引发的,并支持从部分氧化的N-杂环直接进行烷烃脱氢。

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