摘要
The oxidative coupling of methane to C2 hydrocarbons has been studied over a series of La-promoted CaO （La/Ca = 0.05） catalysts, prepared using different precursor salts for CaO and La2O3 （viz. acetates, carbonates, nitrates and hydroxides） and catalyst preparation methods （viz. physical mixing of precursors, co-precipitation using ammonium carbonate/sodium carbonate as a precipitating agent）, under different reaction conditions （temperature： 700-850 ℃, CH4/O2 ratio： 4.0 and 8.0, and GHSV： 51360 cm^3·g^-1·h^- 1）. The surface area and surface basicity/base strength distribution of the catalysts have also been investigated. The surface properties and catalytic activity/selectivity of the La-promoted CaO catalysts vary from catalyst to catalyst depending on the catalyst precursors used and catalyst preparation method. The basicity/base strength distribution is strongly influenced by the precursors （for CaO and La2O3） and catalyst preparation method. Basicity （total and strong basic sites measured in terms of CO2 chemisorbed at 50℃ and 500 ℃, respectively） observed for the catalyst prepared by co-precipitation method is higher than that of the catalysts prepared by physical mixing method. The catalysts prepared by the nitrates of La- and Ca- and co- precipitated by the solution of sodium carbonate and ammonium carbonate exhibit different catalytic performance in OCM. The finding that no direct relationship between the surface basicity and catalytic activity/selectivity in OCM exists indicates that basicity is not solely responsible for obtaining high selectivity to C2 hydrocarbons.
The oxidative coupling of methane to C2 hydrocarbons has been studied over a series of La-promoted CaO （La/Ca = 0.05） catalysts, prepared using different precursor salts for CaO and La2O3 （viz. acetates, carbonates, nitrates and hydroxides） and catalyst preparation methods （viz. physical mixing of precursors, co-precipitation using ammonium carbonate/sodium carbonate as a precipitating agent）, under different reaction conditions （temperature： 700-850 ℃, CH4/O2 ratio： 4.0 and 8.0, and GHSV： 51360 cm^3·g^-1·h^- 1）. The surface area and surface basicity/base strength distribution of the catalysts have also been investigated. The surface properties and catalytic activity/selectivity of the La-promoted CaO catalysts vary from catalyst to catalyst depending on the catalyst precursors used and catalyst preparation method. The basicity/base strength distribution is strongly influenced by the precursors （for CaO and La2O3） and catalyst preparation method. Basicity （total and strong basic sites measured in terms of CO2 chemisorbed at 50℃ and 500 ℃, respectively） observed for the catalyst prepared by co-precipitation method is higher than that of the catalysts prepared by physical mixing method. The catalysts prepared by the nitrates of La- and Ca- and co- precipitated by the solution of sodium carbonate and ammonium carbonate exhibit different catalytic performance in OCM. The finding that no direct relationship between the surface basicity and catalytic activity/selectivity in OCM exists indicates that basicity is not solely responsible for obtaining high selectivity to C2 hydrocarbons.
