Cai An, He Hongwei, Zhang Qicheng, Xu Yongsheng, Li Xintong, Zhang Fengbao, Fan Xiaobin, Peng Wenchao, Li Yang
School of Chemical Engineering and Technology, State Key Laboratory of Chemical Engineering, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin University, Tianjin 300072, People's Republic of China.
ACS Appl Mater Interfaces. 2021 Mar 24;13(11):13087-13096. doi: 10.1021/acsami.0c21177. Epub 2021 Mar 11.
N-doped carbon materials represent a type of metal-free catalyst for diverse organic synthetic reactions. However, single N-doped carbon materials perform insufficiently in the selective oxidation reaction of C-H bond compared with metal catalysts or multielement co-doped materials. There are a few reports on the application of three-dimensional (3D) carbon materials in such a reaction. Besides, the relationship between the well-developed porous structures, heteroatom doping, and their catalytic performance is unclear. In this study, 3D porous N-doped graphene aerogel catalysts with high activity and selectivity for the C-H bond oxidation under mild reaction conditions have been synthesized through a two-step method. Systematic studies on the dosage of N sources, pyrolysis temperature, and their influences on the catalytic performances have been evolved. Moreover, solid evidence of the synergistic effect of sp C atoms adjacent to the N atoms and porous structure promoting the performance has been provided in this work.
氮掺杂碳材料是一类用于多种有机合成反应的无金属催化剂。然而，与金属催化剂或多元素共掺杂材料相比，单一氮掺杂碳材料在C-H键的选择性氧化反应中表现欠佳。关于三维（3D）碳材料在该反应中的应用鲜有报道。此外，发达的多孔结构、杂原子掺杂与其催化性能之间的关系尚不清楚。在本研究中，通过两步法合成了在温和反应条件下对C-H键氧化具有高活性和选择性的3D多孔氮掺杂石墨烯气凝胶催化剂。对氮源用量、热解温度及其对催化性能的影响进行了系统研究。此外，本工作还提供了与氮原子相邻的sp C原子和多孔结构协同促进性能的有力证据。
