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Oxidative coupling of methane over La-promoted CaO catalysts: Influence of precursors and catalyst preparation method
引用本文:Vilas H. Rane,Sopan T. Chaudhari,Vasant R. Choudhary. Oxidative coupling of methane over La-promoted CaO catalysts: Influence of precursors and catalyst preparation method[J]. 天然气化学杂志, 2010, 19(1): 25-30. DOI: 10.1016/S1003-9953(09)60023-2
作者姓名:Vilas H. Rane  Sopan T. Chaudhari  Vasant R. Choudhary
作者单位:Chemical Engineering and Process Development Division,National Chemical Laboratory,Pune 411 008,India 
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 cm3 g-1 h-1)...

关 键 词:催化剂前体  甲烷氧化偶联  制备方法  CaO  La  表面碱性  耦合  强度分布
收稿时间:2009-05-08

Oxidative coupling of methane over La-promoted CaO catalysts: Influence of precursors and catalyst preparation method
Vilas H. Rane,Sopan T. Chaudhari,Vasant R. Choudhary. Oxidative coupling of methane over La-promoted CaO catalysts: Influence of precursors and catalyst preparation method[J]. Journal of Natural Gas Chemistry, 2010, 19(1): 25-30. DOI: 10.1016/S1003-9953(09)60023-2
Authors:Vilas H. Rane  Sopan T. Chaudhari  Vasant R. Choudhary
Affiliation:Chemical Engineering and Process Development Division, National Chemical Laboratory, Pune 411008, India
Abstract:
The oxidative coupling of methane to C2 hydrocarbons has been studied over a series of La-promoted CaO (La/Ca = 0.05) catalysts, preparedusing 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 reactionconditions (temperature: 700–850 ◦C, CH4/O2 ratio: 4.0 and 8.0, and GHSV: 51360 cm3.g−1.h−1). The surface area and surface basicity/basestrength distribution of the catalysts have also been investigated. The surface properties and catalytic activity/selectivity of the La-promotedCaO catalysts vary from catalyst to catalyst depending on the catalyst precursors used and catalyst preparation method. The basicity/basestrength distribution is strongly influenced by the precursors (for CaO and La2O3) and catalyst preparation method. Basicity (total and strongbasic sites measured in terms of CO2 chemisorbed at 50 ◦C and 500 ◦C, respectively) observed for the catalyst prepared by co-precipitationmethod is higher than that of the catalysts prepared by physical mixing method. The catalysts prepared by the nitrates of La- and Ca- and coprecipitatedby the solution of sodium carbonate and ammonium carbonate exhibit different catalytic performance in OCM. The finding that nodirect relationship between the surface basicity and catalytic activity/selectivity in OCM exists indicates that basicity is not solely responsiblefor obtaining high selectivity to C2 hydrocarbons.
Keywords:oxidative coupling of methane  La-promoted CaO catalysts  basicity distribution
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