Mechanistic investigation of the hydrodechlorination of 1,1,1,2-tetrafluorodichloroethane on metal fluoride-supported Pt and Pd |
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| Authors: | Irmina Kris Murwani Erhard Kemnitz Toma
Skapin Mahmood Nickkho-Amiry John M Winfield |
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| Affiliation: | a Institute of Inorganic Chemistry, Humboldt University, Brook-Taylor-Str. 2, D-12489, Berlin, Germany;b Institute “Jo
ef Stefan”, 1000, Ljubljana, Slovenia;c Department of Chemistry, University of Glasgow, Glasgow G12 8QQ, UK |
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| Abstract: | The hydrodechlorination of CF3CCl2F over Pd and Pt supported on β-AlF3 and MgF2 with D2 gas has been investigated employing temperature programmed isotope exchange (TPIE) under static conditions. The isotope exchange observed between the H-loaded metal catalyst and the D2 gas phase demonstrates the significantly higher hydrogen uptake capability of Pd-based catalysts. Both Pd and Pt on β-AlF3, show significantly higher hydrogen/deuterium uptake and isotope exchange activity as compared with the MgF2 support, probably due to the presence of hexagonal channels in β-AlF3 and its higher Lewis acidity. The combination of these properties make Pd/β-AlF3 a superior catalyst for selective hydrodechlorination of CF3CCl2F. Based on the results of the hydrodechlorination of CF3CCl2F with D2, a competitive rather than a consecutive mechanism is proposed. The data from H/D-TPIE are best interpreted by the formation of surface carbene species as intermediates. |
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| Keywords: | Hydrodechlorination of CF3CCl2F Pd and Pt supported on β-AlF3 and MgF2 Deuterium Temperature programmed H/D-isotope exchange Mechanism Surface carbene |
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