Ultrastable 3V-PPh3 polymers supported single Rh sites for fixed-bed hydroformylation of olefins

Miao Jiang, Li Yan, Yunjie Ding, Qi Sun, Jia Liu, Hejun Zhu, Ronghe Lin, Fengshou Xiao, Zheng Jiang, Jingyue Liu

Research output: Contribution to journalArticle

23 Scopus citations

Abstract

The heterogenization of homogeneous catalysts is of critical importance for both fundamental research and practical applications. The key obstacle to industrial applications of heterogenized homogeneous catalysts is the long-term stability of the immobilized molecular complexes. We unambiguously demonstrate in this report that the vinyl-functionalized PPh3 polymers supported single Rh sites (Rh/POL-PPh3) catalyst provided not only excellent catalytic activity but also ultrahigh stability for fixed-bed olefins hydroformylation, which is one of the most important industrial homogeneous catalytic processes for the synthesis of aldehydes and alcohols. HAADF-STEM and EXAFS results indicated that the Rh atoms were present in single Rh sites which were strongly coordinated with the exposed phosphorous atoms of the POL-PPh3 support. The Rh/POL-PPh3 catalyst provided high activity and selectivity because it maintained the catalytic functionalities similar to the homogeneous HRh(CO)(PPh3)3 complex, as demonstrated both by 31P MAS NMR and in situ FT-IR experiments. Thus a reaction mechanism, similar to that over the homogeneous HRh(CO)(PPh3)3 complex, was proposed for olefin hydroformylation over the novel Rh/POL-PPh3 catalyst.

Original languageEnglish (US)
Pages (from-to)211-217
Number of pages7
JournalJournal of Molecular Catalysis A: Chemical
Volume404-405
DOIs
StatePublished - May 30 2015

Keywords

  • Heterogenized catalysts
  • Hydroformylation
  • Porous organic ligands
  • Rhodium
  • Stability

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology
  • Physical and Theoretical Chemistry

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