Vapor-phase ethanol carbonylation with heteropolyacid-supported Rh

Sara Yacob, Sunyoung Park, Beata A. Kilos, David G. Barton, Justin M Notestein

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

Ethanol carbonylation is a potential route to valuable C3 products. Here, Rh supported on porous, Cs-exchanged heteropolyacid Cs3PW12O40, is demonstrated as an effective catalyst for vapor-phase ethanol carbonylation, with higher selectivity and conversion to propionates than existing catalysts. Residual acidity or a Mo polyatom was strongly detrimental to yields. Propionate selectivity was maximized at 96% at 170 °C and with added H2O. The catalyst displayed stable selectivity over 30 h on stream and up to 77% conversion. Ethyl iodide is a required co-catalyst but at levels as low as 2% relative to ethanol. XPS and in situ XANES indicate partial Rh reduction, consistent with the formation of low-valent reactive intermediates and slow deactivation through formation of Rh nanoparticles. With further optimization and understanding, these Rh/heteropolyacid catalysts may lead to stable and selective catalysts for the production of propionates through ethanol carbonylation.

Original languageEnglish
Pages (from-to)1-8
Number of pages8
JournalJournal of Catalysis
Volume325
DOIs
Publication statusPublished - May 1 2015

Fingerprint

Carbonylation
Ethanol
ethyl alcohol
Vapors
vapor phases
catalysts
Catalysts
Propionates
Catalyst selectivity
selectivity
Iodides
Acidity
acidity
deactivation
iodides
X ray photoelectron spectroscopy
routes
Nanoparticles
nanoparticles
optimization

Keywords

  • Carbonylation
  • Ethanol
  • Heteropolyacid
  • Iodide
  • Rhodium

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

Vapor-phase ethanol carbonylation with heteropolyacid-supported Rh. / Yacob, Sara; Park, Sunyoung; Kilos, Beata A.; Barton, David G.; Notestein, Justin M.

In: Journal of Catalysis, Vol. 325, 01.05.2015, p. 1-8.

Research output: Contribution to journalArticle

Yacob, Sara ; Park, Sunyoung ; Kilos, Beata A. ; Barton, David G. ; Notestein, Justin M. / Vapor-phase ethanol carbonylation with heteropolyacid-supported Rh. In: Journal of Catalysis. 2015 ; Vol. 325. pp. 1-8.
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