Catalysis Letters, Vol.69, No.1-2, 43-50, 2000
A comparative study of reactions of methanol over catalysts derived from NiAl- and CoAl-layered double hydroxides and their Sn-containing analogues
Ni- and Co-based catalysts derived from NiAl- and CoAl-layered double hydroxides were tested in four kinds of reactions of methanol, namely decomposition of methanol (DCM), partial oxidation of methanol (POM), steam reforming of methanol (SRM), and oxidative steam reforming of methanol (OSRM), for the purpose of H-2 production for fuel cells. H-2, CO and/or CO2 were the predominant products with minor amounts of dimethyl ether (DME) and CH4 depending on the reaction temperature. Among the four kinds of reactions tested, the OSRM reaction was found to be more effective in terms of MeOH conversion and H-2 selectivity over these catalysts. Higher selectivity of H-2 and CO2 with only traces of CO could be obtained at about 100% methanol conversion around 300 C-degrees in the OSRM reaction over the catalyst derived from CoAl-LDH. Substitution of a part of Al by Sn in the NiAl- and CoAl-LDH systems was found to be inhibiting the methanol conversion. On the other hand, the selectivities to DME and CH4 were declined with a consequent increase in the selectivity to H-2. In addition, considerable amount of formaldehyde was also noticed, especially over the catalyst derived from CoAlSn-LDH at lower reaction temperatures. The observed difference in the catalytic performance upon Sn incorporation was attributed to an improved redox capability of the Ni- and Co-based oxide catalysts, as determined by temperature-programmed reduction (TPR) experiments.
Keywords:methanol reactions;hydrogen production;partial oxidation of methanol;steam reforming of methanol;Ni-based catalysts;Co-based catalysts;layered double hydroxides