Isotopic transient techniques were applied to study oxidative coupling of methane over lanthanum oxide and strontium promoted La2O3 catalysts. Results of the18O2/16O2 isotopic exchange experiments indicate that Sr promotion increases oxygen uptake from the lattice of the catalyst. Oxygen self diffusion coefficients, which were determined for the series of lanthana catalysts, reach a maximum for the 1% Sr/La2O3. Steps of18O2 in the presence of a steady flow of methane over Sr/La2O3 catalysts, indicate that surface and bulk oxygen appear in the reaction products before gas-phase18O2. Steps of CO2 over catalysts in which lattice oxygen has been exchanged with18O2, show that gas/solid exchange involves over 50% of the lattice oxygen. Under reaction conditions, methane pulses with no gas-phase oxygen yield negligible amounts of products which indicates that methane interacts with lattice oxygen only in the presence of the gas-phase oxygen. 相似文献
Li-doped sulfated-zirconia catalysts were found to be effective for oxidative coupling of methane (OCM). The catalyst performances depend on the sulfate content and calcination temperature. A maximum C2 yield is attained over the catalysts, which contain 6 wt.% sulfate and calcined at 923–973 K, being closely related to the preparation conditions of sulfated-ZrO2 as solid super-acids. When the performances of the Li-doped sulfated-ZrO2 (Li/SZ) catalysts were tested at 1023 K as a function of reaction time, both the C2 and COx selectivities remained constant over the range of 8 h, but the CH4 conversion decreased from 17.5% to 11.9%. The nature of Li/SZ catalysts for the OCM was investigated by X-ray diffraction, XPS, and NH3 and CO2 TPD measurements. It could be postulated that the sulfated-ZrO2 surface could play an important role in the formation of a catalytically active structure by Li-doping. 相似文献
The oxidative coupling of methane (OCM) has been found to be structure sensitive on La2O3 catalysts exhibiting different crystallite morphologies. Thin plates obtained by thermal decomposition of lanthanum nitrate at 650 °C are more selective on OCM reaction performed at 750 °C than the particles obtained by decomposition of the nitrate at 800 °C. It is assumed that the oxycarbonate observed is formed from the methane deep oxidation on the catalyst surface. This compound appears to act as an intermediate in the production of CO2 and is thus important hi the resulting selectivity. 相似文献
Imidazolium bromide-based ionic liquids bearing phosphonyl groups on the cationic part were synthesized and grafted on γ-alumina (γ-Al2O3) powders. These powders were prepared as companion samples of conventional mesoporous γ-alumina membranes, in order to favor a possible transfer of the results to supported membrane materials, which could be used for CO2 separation applications. Effective grafting was demonstrated using energy dispersive X-ray spectrometry (EDX), N2 adsorption measurements, fourier transform infrared spectroscopy (FTIR), and special attention was paid to 31P and 13C solid state nuclear magnetic resonance spectroscopy (NMR). 相似文献
A simple N‐heterocyclic carbene (NHC) derived from 1‐methyl‐3‐ethylimidazolium tetrafluoroborate was found to be an efficient ligand for a range of copper‐catalyzed cross‐coupling reactions, leading to the formation of aromatic ethers and thioethers.