催化作用
苯乙炔
材料科学
介孔材料
氮气
化学工程
兴奋剂
纳米技术
组合化学
有机化学
化学
光电子学
工程类
作者
Qian Zhang,Zhilin Liu,Shaohang Zheng,Luoqi Wang,Ling Zhang,Zhen‐An Qiao
标识
DOI:10.1002/adma.202209635
摘要
Supported metal catalysts have played an important role in optimizing selective semihydrogenation of alkynes for fine chemicals. There into, nitrogen-doped carbons, as a type of promising support materials, have attracted extensive attentions. However, due to the general phenomenon of random doping for nitrogen species in the support, it is still atremendous challenge to finely identify which nitrogen configuration dominates the catalytic property of alkynes' semihydrogenation. Herein, it is reported that uniform mesoporous N-doped carbon spheres derived from mesoporous polypyrrole spheres are used as supports to immobilized subnanometric Pd clusters, which provide a particular platform to research the influence of nitrogen configurations on the alkynes' semihydrogenation. Comprehensive experimental results and density functional theory calculation indicate that pyridinic nitrogen configuration dominates the catalytic behavior of Pd clusters. The high contents of pyridinic nitrogen sites offer abundant coordination sites, which greatly reduces the energy barrier of the rate-determining reaction step and makes Pd clusters own high catalytic activity. The electron effect between pyridinic nitrogen sites and Pd clusters makes the reaction highly selective. Additionally, the good mesostructures also promote the fast transport of substrate. Based on the above, catalyst Pd@PPy-600 exhibits high catalytic activity (99%) and selectivity (96%) for phenylacetylene (C8 H6 ) semihydrogenation.
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