Catalytically Active Co−Nx Species Stabilized on Nitrogen‐doped Porous Carbon for Efficient Hydrogenation and Dehydrogenation of N‐heteroarenes,ChemCatChem

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Catalytically Active Co−Nx Species Stabilized on Nitrogen‐doped Porous Carbon for Efficient Hydrogenation and Dehydrogenation of N‐heteroarenes
ChemCatChem ( IF 3.8 ) Pub Date : 2020-05-26 , DOI: 10.1002/cctc.202000826
Dan Xu ₁ , Hong Zhao ₁ , Zhengping Dong ₁ , Jiantai Ma ₁

Affiliation

The development of bifunctional, highly active and stable non‐noble‐metal catalysts is important for synthetic chemistry. In this study, a highly dispersed Co catalyst stabilized on the mesoporous N‐doped carbon layers was prepared by adsorption and pyrolysis of cobalt complex on dendritic fibrous silica nanospheres (KCC‐1@Co−N−C−T). The characterizations of HAADF‐STEM, XRD and XPS together with the KSCN poisoning tests determine the absence of Co⁰ or CoO_x nanoparticles and suggest that the Co−N_x species are the active sites. The formation of Co−N_x species results from the properties of N‐rich cobalt‐phenanthroline complex and dendritic fibrous silica supports, increasing the original spatial distance between Co atoms and thus preventing them from aggregation. The KCC‐1@Co−N−C‐800 catalyst showed excellent activity and selectivity for the oxidative dehydrogenation (ODH) of saturated N‐heterocycles and base‐free catalytic transfer hydrogenation (CTH) of unsaturated N‐heterocycles.

中文翻译：

在氮掺杂的多孔碳上稳定的催化活性Co-Nx物种，用于N-杂芳烃的有效加氢和脱氢

开发双功能，高活性和稳定的非贵金属催化剂对于合成化学非常重要。在这项研究中，通过在树枝状纤维状二氧化硅纳米球（KCC-1 @ Co-N-C-T）上吸附和热解钴络合物，制备了稳定分散在中孔N掺杂碳层上的高分散Co催化剂。HAADF‐STEM，XRD和XPS的特征以及KSCN中毒测试确定了Co ⁰或CoO _x纳米颗粒的缺失，并表明Co-N _x物种是活性位点。Co-N _x的形成物种是由富含N的钴菲咯啉配合物和树枝状纤维状二氧化硅载体产生的，从而增加了Co原子之间的原始空间距离，从而阻止了它们的聚集。KCC-1 @ Co-N-C-800催化剂对饱和N-杂环的氧化脱氢（ODH）和不饱和N-杂环的无碱催化转移氢化（CTH）表现出出色的活性和选择性。

更新日期：2020-05-26

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