• 文献标题:   Preserved in a Shell: High-Performance Graphene-Confined Ruthenium Nanoparticles in Acetylene Hydrochlorination
  • 文献类型:   Article
  • 作  者:   KAISER SK, LIN RH, KRUMEICH F, SAFONOVA OV, PEREZRAMIREZ J
  • 作者关键词:   acetylene hydrochlorination, catalyst lifetime, graphene, nanostructuring, ruthenium nanoparticle
  • 出版物名称:   ANGEWANDTE CHEMIEINTERNATIONAL EDITION
  • ISSN:   1433-7851 EI 1521-3773
  • 通讯作者地址:   Swiss Fed Inst Technol
  • 被引频次:   9
  • DOI:   10.1002/anie.201906916 EA JUL 2019
  • 出版年:   2019

▎ 摘  要

The potential implementation of ruthenium-based catalysts in polyvinyl chloride production via acetylene hydrochlorination is hindered by their inferior activity and stability compared to gold-based systems, despite their 4-fold lower price. Combining in-depth characterization and kinetic analysis we reveal the superior activity of ruthenium nanoparticles with an optimal size of 1.5 nm hosted on nitrogen-doped carbon (NC) and identify their deactivation modes: 1) nanoparticle redispersion into inactive single atoms and 2) coke formation at the metal sites. Tuning the density of the NC carrier enables a catalytic encapsulation of the ruthenium nanoparticles into single layer graphene shells at 1073 K that prevent the undesired metal redispersion. Finally, we show that feeding O-2 during acetylene hydrochlorination limits coke formation over the nanodesigned ruthenium catalyst, while the graphene layer is preserved, resulting in a stability increase of 20 times, thus rivalling the performance of gold-based systems.