沉淀剂对SrCO3/La2O2CO3上低温甲烷氧化偶联反应的影响
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TQ 032. 4

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The effects of the precipitators on the low-temperature oxidative coupling of methane over SrCO3/La2O2CO3 catalysts and the thermal effects in the reaction
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    摘要:

    利用共沉淀法制备了系列SrCO3/La2O2CO3催化剂,制备中沉淀剂的选择影响催化剂的物理化学性质,并最终决定其在低温甲烷氧化偶联(OCM)中的催化性能,其中以摩尔比2:1的NaOH/Na2CO3 为复合沉淀剂效果最好,对应的催化剂中检测到两种La2O2CO3的组分,分别为四方晶相的(I-)和六方晶相的(II-)La2O2CO3。这两种晶相的共存为OCM的低温反应提供所需要的活性位。助剂SrCO3 抑制了甲烷的过度氧化,提高了C2的选择性。所得到的最佳的催化剂能在100 oC炉温下维持OCM反应至少24 h,使CH4.转化率达到25.6%,C2选择性达到43.4%。伴随OCM的甲烷氧化生成COx的副反应产生的热点效应为OCM温和反应提供了热源。

    Abstract:

    A series of SrCO3/La2O2CO3 catalysts prepared by thermal decomposition and co-precipitation method were tested in low-temperature OCM (oxidative coupling of methane). The choice of precipitators played great role on the catalytic performance, and the catalysts obtained by the multiple precipitators NaOH/Na2CO3 showed better activity and stability than the catalysts obtained by single precipitator. Both tetragonal (I-) and hexagonal (II)-La2O2CO3 was detected in the catalysts, and their coexistence provided two types of active sites for OCM to produce C2 and deep oxidation of methane to produce COx, respectively. The later reaction was high exothermic, which provided the hot spot for the ignition of the OCM reaction, and great energy to maintain the reaction. The catalyst with 25 mol.% of SrCO3 could hold the reaction for at least 24 h at Tex=100 oC (external furnace temperature) with CH4 conversion of 25.6% and C2 selectivity of 43.4%.

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张军.沉淀剂对SrCO3/La2O2CO3上低温甲烷氧化偶联反应的影响[J].精细化工,2010,27(4):

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  • 收稿日期:2009-12-07
  • 最后修改日期:2009-12-30
  • 录用日期:2010-01-06
  • 在线发布日期: 2010-01-26
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