Increased productivity in ethylene carbonylation by zeolite-supported molybdenum carbonyls

Chieh Chao Yang, Sara Yacob, Beata A. Kilos, David G. Barton, Eric Weitz, Justin M. Notestein

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

Ethylene carbonylation to propionic acid is a powerful route to the synthesis of oxygenates. Mo(CO)6 is a known homogenous catalyst for this reaction. When supported on HY zeolite, prepared by incipient wetness impregnation from pentane or by vapor deposition, turnover numbers dramatically increase to over 40,000 in 5 h of reaction, particularly for the supports with lower Si/Al ratios. Diffuse reflectance UV-visible spectra and thermogravimetric analysis indicate that lower Si/Al ratios promote more and stronger interactions between Mo(CO)6 and the support, leading to higher reactivity under liquid-phase reaction conditions. Although some leaching occurs under these conditions, the active catalyst is the supported Mo(CO)x/HY, and the recovered catalysts are still stable and active for ethylene carbonylation with turnover numbers exceeding 30,000 mol propionic acid/mol of Mo over 5 h at 190 °C. FTIR provides evidence for the formation and stabilization of under-coordinated carbonyl species during heat treatment, and such sub-carbonyls are known to be relevant in previously-established catalytic mechanisms.

Original languageEnglish
Pages (from-to)313-320
Number of pages8
JournalJournal of Catalysis
Volume338
DOIs
Publication statusPublished - Jun 1 2016

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Keywords

  • Carbonylation
  • Ethylene
  • Heterogeneous catalysis
  • Impregnation
  • Metal carbonyl
  • Molybdenum
  • Promotion
  • Y-type zeolite

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

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