O. Garnier et al., MEMBRANE-ASSISTED 2-STEP PROCESS FOR METHANE CONVERSION INTO HYDROGENAND HIGHER HYDROCARBONS, Industrial & engineering chemistry research, 36(3), 1997, pp. 553-558
In this work, methane conversion was carried out over a group VIII met
al in a Pd-Ag membrane reactor to produce hydrogen and higher hydrocar
bons in a nonoxidative atmosphere. A two-step reaction sequence operat
ed at two different temperatures was adopted to pass around the thermo
dynamic barrier of low-temperature methane conversion. Methane was fir
st activated as a result of the dissociative deposition over a Ru cata
lyst, followed by rehydrogenation to form higher hydrocarbons. The use
of the Pd-Ag membrane reactor significantly enhanced the methane conv
ersion into hydrogen and carbonaceous species in the first step and th
e yield of higher hydrocarbons upon rehydrogenation in the second step
. The repartition of different carbonaceous species was monitored by t
emperature-programed surface reaction(TPSR). The effective methane con
version at low temperatures in the membrane reactor favored the format
ion of C-alpha species which were selective to produce higher hydrocar
bons. A C-2+ yield of about 16% was obtained by conducting methane dec
omposition at 300 degrees C and rehydrogenation at 100-120 degrees C i
n the Pd-Ag membrane reactor.