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《CHINESE JOURNAL OF CATAL YSIS》 1994-05
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OXIDATIVE COUPLING OF METHANE OVER ACCEPTOR-DOPED CaTiO_3

Yu, Chun-ying; Li, Wen-zhao and Qi, Ai-hua(Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023)  
The partial substitution of acceptor impurities (Al3+, Mg2+, Li+)for Ti4+ in perovskite SrTiO3 could result in a significant improvementof C2 selectivity for oxidative coupling of methane (OCM) and a good relationship between the C,selectivity and the p-type semiconductivity ofthe doped SrTiO3 has been found. It was found in this paper that partialsubstitution of acceptor impurities (Al3+, Mg2+, Li+ ) for Ti4+ inCaTiO3 could also result in a significant improvement both for C2 selectivity of OCM and for p-type semiconductivity. The highest C2 yield wasobserved for CaTi0.9 Li0.1 O3-δ catalyst which gave CH, conversion 35.7 %with a C2 hydrocarbons selectivity of 53. 9% at 750℃. XPS and TPRmeasurements showed that non-fully-reduced oxygen species Oδ- (oδ2) existed on doped CaTiO3, which was created by interaction between lattice oxygen and h' in valence band of the p-type semiconductor. CH4 reaction with lattice oxygen of catalyst showed that lattice oxygen O2- was responsible for complete oxidation of CH4 and non-fully-reduced oxygen species Oδ- was responsible for oxidative coupling of CH4.Li in CaTi0.9 Li0.1 O3-δ was more stable than that in Li-doped metal oxidecatalysts, such as Li/MgO and Li/TiO2.
【Fund】: 国家自然科学基金
【CateGory Index】: O621.254.1
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