Journal of the Electrochemical Society, Vol.144, No.1, 1-5, 1997
Selective Oxidation of Ethane Using the Au-Vertical-Bar-YSZ-Vertical-Bar-Ag Electrochemical Membrane System
The catalytic conversion of ethane to acetaldehyde on an inert gold electrode has been studied using the electrochemical membrane reactor with yttria-stabilized zirconia (YSZ) solid electrolyte at 475 degrees C. On applying a direct current to the reaction cell, 5% ethane in N-2, AuYSZAg, 100% O-2, acetaldehyde was formed and the formation rate increased linearly with increasing current. Selectivities to acetaldehyde and carbon dioxide were 45 and 55%, respectively. The addition of oxygen to the ethane-mixed gas in the anode space did not affect the acetaldehyde formation. The use of YSZ powder as a fixed bed catalyst under the mixed gas flow of ethane and oxygen at 450 to 600 degrees C resulted in the formation of carbon monoxide, carbon dioxide, and ethene. Even the use of N2O instead of oxygen resulted in no formation of acetaldehyde. Hence, it is likely that partial oxidation of ethane to acetaldehyde was carried out by the oxygen species transferred electrochemically through the YSZ which appeared at the gold-YSZ-gas triple-phase boundary. From the results of ethanol oxidation over the AuYSZAg system, the following mechanism was proposed : ethane is dehydrogenated to an ethyl radical, then converted to ethoxide, and finally to acetaldehyde by the oxygen species transferred through the YSZ.
Keywords:YTTRIA-STABILIZED ZIRCONIA;NITROUS-OXIDE;DEHYDROGENATION;CATALYSTS;ZRO2;ACETALDEHYDE;MOLYBDENUM;VANADIUM;KINETICS;ETHYLENE