Bifunctional Organorhodium Solid Acid Catalysts for Methanol Carbonylation

Robust, bifunctional catalysts comprising Rh(CO)(Xantphos) exchanged phosphotungstic acids of general formulas [Rh(CO)(Xantphos)]+ n [H3–n PW12O40] n− have been synthesized over silica supports which exhibit tunable activity and selectivity toward direct vapor phase methanol carbonylation. The optim...

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Bibliographic Details
Published in:ACS catalysis 2012-07, Vol.2 (7), p.1368-1376
Main Authors: Dingwall, Lee D, Lee, Adam F, Lynam, Jason M, Wilson, Karen, Olivi, Luca, Deeley, Jon M. S, Gaemers, Sander, Sunley, Glenn J
Format: Article
Language:English
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Summary:Robust, bifunctional catalysts comprising Rh(CO)(Xantphos) exchanged phosphotungstic acids of general formulas [Rh(CO)(Xantphos)]+ n [H3–n PW12O40] n− have been synthesized over silica supports which exhibit tunable activity and selectivity toward direct vapor phase methanol carbonylation. The optimal Rh:acid ratio = 0.5, with higher rhodium concentrations increasing the selectivity to methyl acetate over dimethyl ether at the expense of lower acidity and poor activity. On-stream deactivation above 200 °C reflects Rh decomplexation and reduction to Rh metal, in conjunction with catalyst dehydration and loss of solid acidity because of undesired methyl acetate hydrolysis, but can be alleviated by water addition and lower temperature operation.
ISSN:2155-5435
2155-5435
DOI:10.1021/cs3000528