Developing new heterogeneous non-noble metal catalysts to replace noble-metal catalysts in organic transformations is of high importance in modern synthetic chemistry. Herein, nitrogen-doped carbon embedded Co catalysts (abbreviated as Co@CN-T-AT, in which T represents the pyrolysis temperature, AT represents the acid-leaching process) were prepared through the simple pyrolysis of graphene oxide-supported cobalt-based zeolitic imidazolate-frameworks, followed by the acid-leaching process. The Co@CN-600-AT catalyst demonstrated the highest catalytic activity among the synthesized Co catalyst toward the reductive amination of carbonyl compounds with nitro compounds by transfer hydrogenation with formic acid as the hydrogen donor, which integrated three consecutive steps into a one-pot reaction. By applying this catalyst, structurally diverse secondary amines were produced in good to excellent yields without the reduction of other functional groups. The transfer hydrogenation of the imines (C═N bonds) was the rate-determining step. Furthermore, the catalyst was highly stable and could be reused without decrease of the catalytic activity.

中文翻译：

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耐酸钴催化剂上以甲酸为氢供体的一锅还原胺化合成仲胺

在现代合成化学中，开发新的非均相非贵金属催化剂来替代有机转化中的贵金属催化剂非常重要。在此，通过对氧化石墨烯负载的钴基钴进行简单的热解，制备了氮掺杂的碳包埋Co催化剂（简称Co @ CN-T-AT，其中T代表热解温度，AT代表酸浸过程）。沸石咪唑酸盐骨架，然后进行酸浸过程。Co @ CN-600-AT催化剂在合成的Co催化剂中表现出最高的催化活性，该方法通过将甲酸作为氢供体转移加氢反应，将羰基化合物与硝基化合物还原胺化反应，该反应将三个连续的步骤整合到一个罐中反应。通过使用这种催化剂，在不降低其他官能团的情况下，以良好至极好的收率生产出结构多样的仲胺。亚胺（C═N键）的转移氢化是决定速率的步骤。此外，该催化剂是高度稳定的，并且可以在不降低催化活性的情况下重复使用。