Controlling N-doping type in carbon to boost single-atom site Cu catalyzed transfer hydrogenation of quinoline
nitrogen-doping type, metal oxide, nitrogen-doped carbon, single-atom site catalyst, transfer hydrogenation
Single-atom site (SA) catalysts on N-doped carbon (CN) materials exhibit prominent performance for their active sites being M-Nx. Due to the commonly random doping behaviors of N species in these CN, it is a tough issue to finely regulate their doping types and clarify their effect on the catalytic property of such catalysts. Herein, we report that the N-doping type in CN can be dominated as pyrrolic-N and pyridinic-N respectively through compounding with different metal oxides. It is found that the proportion of distinct doped N species in CN depends on the acidity and basicity of compounded metal oxide host. Owing to the coordination by pyrrolic-N, the SA Cu catalyst displays an enhanced activity (two-fold) for transfer hydrogenation of quinoline to access the valuable molecule tetrahydroquinoline with a good selectivity (99%) under mild conditions. The higher electron density of SA Cu species induced by the predominate pyrrolic-N coordination benefits the hydrogen transfer process and reduces the energy barrier of the hydrogenation pathway, which accounts for the improved catalytic effeciency.
Tsinghua University Press
Jian Zhang,Caiyan Zheng,Maolin Zhang,Yajun Qiu,Qi Xu,Weng-Chon Cheong,Wenxing Chen,Lirong Zheng,Lin Gu,Zhengpeng Hu,Dingsheng Wang,Yadong Li, Controlling N-doping type in carbon to boost single-atom site Cu catalyzed transfer hydrogenation of quinoline. NanoRes.2020, 13(11): 3082–3087