TY - JOUR
T1 - Mechanistic investigation of the hydrodechlorination of 1,1,1,2-tetrafluorodichloroethane on metal fluoride-supported Pt and Pd
AU - Murwani, Irmina Kris
AU - Kemnitz, Erhard
AU - Skapin, Tomaž
AU - Nickkho-Amiry, Mahmood
AU - Winfield, John M.
PY - 2004/2/15
Y1 - 2004/2/15
N2 - 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.
AB - 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.
KW - Deuterium
KW - Hydrodechlorination of CFCClF
KW - Mechanism
KW - Pd and Pt supported on β-AlF and MgF
KW - Surface carbene
KW - Temperature programmed H/D-isotope exchange
UR - http://www.scopus.com/inward/record.url?scp=0742267139&partnerID=8YFLogxK
U2 - 10.1016/j.cattod.2003.11.011
DO - 10.1016/j.cattod.2003.11.011
M3 - Article
AN - SCOPUS:0742267139
SN - 0920-5861
VL - 88
SP - 153
EP - 168
JO - Catalysis Today
JF - Catalysis Today
IS - 3-4
ER -