催化作用
离子键合
化学
吸附
乙炔
阳离子聚合
选择性
钯
光化学
无机化学
材料科学
物理化学
高分子化学
有机化学
离子
作者
Xingju Li,Hua Wang,Qiao Yuan,Xinshan Song,Jiali Mu,Wei Yao,Yan Li,Fanfei Sun,Siquan Feng,Yuyang Cai,Zheng Jiang,Zhongkang Han,Yunjie Ding
标识
DOI:10.1002/anie.202307570
摘要
Heterogeneous single-metal-site catalysts usually suffer from poor stability, thereby limiting industrial applications. Dual Pd1 -Ru1 single-atom-sites supported on porous ionic polymers (Pd1 -Ru1 /PIPs) were constructed using a wetness impregnation method. The two isolated metal species in the form of a binuclear complex were immobilized on the cationic framework of PIPs through ionic bonds. Compared to the single Pd- or Ru-site catalyst, the dual single-atom system exhibits higher activity with 98 % acetylene conversion and near 100 % selectivity to dialkoxycarbonylation products, as well as better cycling stability for ten cycles without obvious decay. Based on DFT calculations, it was found that the single-Ru site exhibited a strong CO adsorption energy of -1.6 eV, leading to an increase in the local CO concentration of the catalyst. Notably, the Pd1 -Ru1 /PIPs catalyst had a much lower energy barrier of 2.49 eV compared to 3.87 eV of Pd1 /PIPs for the rate-determining step. The synergetic effect between neighboring single sites Pd1 and Ru1 not only enhanced the overall activity, but also stabilized PdII active sites. The discovery of synergetic effects between single sites can deepen our understanding of single-site catalysts at the molecular level.
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