Hollow periodic mesoporous organosilica spheres (HPMOs) have stimulated great research interest owing to its unique organic–inorganic hybrid skeleton. In this work, HPMOs were synthesized by hydrothermal method, and then cobalt and nitrogen co-doped carbon catalyst was prepared by using HPMOs as supports. The optimal catalyst (Co-Nx/HPMOs-D) performed excellent activity in the selective oxidation reaction of aryl alkanes, with the conversion of ethylbenzene up to 97.0% and the selectivity of acetophenone was 98.9%, which was attributed to the Co-Nx active species and the unique HPMOs supports. The unique amphiphilic property of Co-Nx/HPMOs-D could better facilitate the adsorption and diffusion of organic substrates in the aqueous phase. The addition of dicyandiamide not only enhanced the nitrogen content in the catalyst, but also promoted the conversion of pyrrolic-N to pyridinic-N during the pyrolysis process, thus strengthened the interaction between the substrate and cobalt and improved the stability of the catalyst. This work presented a green and environmentally friendly method for the preparation of HPMOs and a facile strategy to obtain high performance catalysts for selective oxidation of aryl alkanes.

中文翻译：

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钴氮共改性空心周期性介孔有机硅球用于芳基烷烃的选择性氧化

中空周期性介孔有机硅球（HPMO）由于其独特的有机-无机杂化骨架而引起了人们极大的研究兴趣。本工作采用水热法合成了HPMOs，并以HPMOs为载体制备了钴氮共掺杂碳催化剂。最优催化剂(Co-Nx/HPMOs-D)在芳烷烃选择氧化反应中表现出优异的活性，乙苯转化率高达97.0%，苯乙酮选择性为98.9%，这归功于Co-Nx活性物质和独特的 HPMO 支持。 Co-Nx/HPMOs-D独特的两亲特性可以更好地促进有机底物在水相中的吸附和扩散。双氰胺的加入不仅提高了催化剂中的氮含量，而且促进了热解过程中吡咯-N向吡啶-N的转化，从而加强了基质与钴之间的相互作用，提高了催化剂的稳定性。这项工作提出了一种绿色环保的 HPMO 制备方法，以及一种获得高性能芳烷烃选择性氧化催化剂的简便策略。