• 文献标题:   Polymeric Ruthenium Porphyrin-Functionalized Carbon Nanotubes and Graphene for Levulinic Ester Transformations into gamma-Valerolactone and Pyrrolidone Derivatives
  • 文献类型:   Article
  • 作  者:   ZHANG T, GE Y, WANG XF, CHEN JZ, HUANG XL, LIAO YN
  • 作者关键词:  
  • 出版物名称:   ACS OMEGA
  • ISSN:   2470-1343
  • 通讯作者地址:   Jinan Univ
  • 被引频次:   14
  • DOI:   10.1021/acsomega.7b00427
  • 出版年:   2017

▎ 摘  要

Polymeric ruthenium porphyrin-functionalized carbon nanotubes (Ru-PP/CNTs) were prepared by the metallation of polymeric porphyrinfunctionalized carbon nanotubes (PP/CNTs) with Ru-3(CO)(12), whereas PP/CNTs were obtained by the condensation of terephthaldehyde and pyrrole in the presence of CNTs. The Ru-PP/CNTs have a thin layer of highly cross-linked polymeric ruthenium porphyrin coating over the CNT surface via strong p-p stacking interactions, thus showing a bilayered structure with an amorphous polymeric outer surface and an internal CNT core. Polymeric ruthenium porphyrin-functionalized reduced graphene oxide (Ru-PP/RGO) was prepared with a synthetic procedure similar to Ru-PP/CNTs, with RGO as the internal core. Both Ru-PP/CNTs and Ru-PP/RGO showed excellent catalytic performance toward hydrogenation of biomass-related ethyl levulinate (EL) to gamma-valerolactone (GVL) with Ru-centered porphyrin units as the catalytic active species. Under optimized reaction conditions, a GVL yield higher than 99% with a complete conversion of EL was observed over both Ru-PP/CNTs and Ru-PP/RGO. In addition to GVL preparation, the versatile Ru-PP/ CNTs can efficiently promote reductive amination of EL with various amines for the synthesis of pyrrolidone derivatives, with the corresponding yields ranging from 96.3 to 88.7%. Moreover, the composite materials of both Ru-PP/CNTs and Ru-PP/RGO behave as heterogeneous catalysts in the reaction system and can be easily reused.