化学
催化作用
甲烷氧化偶联
甲烷
X射线光电子能谱
钙钛矿(结构)
选择性
氧化态
无机化学
相(物质)
多相催化
结晶学
化学工程
有机化学
工程类
作者
Tinku Baidya,Niels van Vegten,René Verel,Yijiao Jiang,Maxim Yulikov,Thomas D. Kohn,Gunnar Jeschke,Alfons Baiker
标识
DOI:10.1016/j.jcat.2011.05.005
摘要
Varying the composition of Sr–Al oxides, mixed as well as single phase compounds were prepared and characterized extensively by XRD, NMR, TEM, EPR, XPS, and TPD. Depending on synthesis method and precursors, Sr/Al-based materials with different crystalline phases (e.g., Sr3Al4O9·2H2O, double perovskite, SrAl4O7, SrAl2O4, and SrCO3) were obtained. Apart from these crystalline phases, several other species were present, as identified by solid state NMR and TG–MS. The ratio of tetrahedrally to octahedrally coordinated Al (AlIV/AlVI) in the Sr/Al mixed oxides increased from 0.5 (pure alumina) to 5.2 in Sr/Al = 1.25, as determined by solid state NMR. The performance of these catalysts in the oxidative coupling of methane depended on the AlIV/AlVI ratio, both activity as well as C2+ selectivity increased with increasing Sr-content. The catalyst with a Sr/Al ratio of 1.25 showed a performance comparable to the well-known catalyst 1.9%Mn–4%Na2WO4/SiO2 under the conditions used (810 °C, CH4:O2 = 108:22, GHSV ∼ 26,000 L/kgcat h).
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