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Oxidative coupling of methane over alkaline earth oxides deposited on commercial support precoated with rare earth oxides

机译:甲烷在碱土金属氧化物上的氧化偶联,碱土金属氧化物沉积在预先涂有稀土氧化物的商业载体上

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摘要

A number of supported catalysts, prepared by depositing alkaline earth (viz. Mg, Ca, Sr and Ba) oxides on a commercial support (SA- 5205) precoated with various rare earth (viz. La, Ce, Nd, Sm, Gd, Er and Yb) oxides have been evaluated for their surface properties and activity/selectivity in oxidative coupling of methane (OCM) at low contact time (GHSV = 1.02 × 10~5 cm~3 g~(-1) h~(-1)). The catalysts have been characterized for their basicity and acidity distributions by temperature programmed desorption (TPD) Of CO_2 and ammonia from 50 deg C to 950 deg C, respectively, and for their oxygen chemisorption sites by TPD of O_2. The OCM activity of the catalysts has been correlated with their basic sites measured in terms of the CO_2 desorbed between 500 deg C and 950 deg C. The catalysts with La_2O_3 and/or Nd_2O_3, showing good OCM activity, have been compared for their performance in the OCM process at different temperatures (750 deg C-850 deg C), and CH_4/O_2 ratios (4.0- 20.0) in the feed. At 850 deg C, the catalyst with SrO deposited on the support precoated with mixed La_2O_3-Nd_2O_3 shows best performance in the OCM process.
机译:通过在预先涂有各种稀土金属(例如La,Ce,Nd,Sm,Gd)的商品化载体(SA-5205)上沉积碱土金属氧化物(即Mg,Ca,Sr和Ba)氧化物而制得的许多载体催化剂,已对Er和Yb)氧化物在低接触时间(GHSV = 1.02×10〜5 cm〜3 g〜(-1)h〜(-1)下的甲烷氧化偶联(OCM)的表面性质和活性/选择性进行了评估))。催化剂的特征在于它们的碱度和酸度分布分别是从50℃到950℃的CO_2和氨的程序升温脱附(TPD),以及它们的O_2的TPD对氧的化学吸附位点。催化剂的OCM活性已与其在500℃至950℃之间解吸的CO_2的碱性位点相关联。比较了La_2O_3和/或Nd_2O_3表现出良好的OCM活性的催化剂的性能。在不同温度(750℃至850℃)和进料中CH_4 / O_2比(4.0-20.0)下进行OCM处理。在850摄氏度下,具有SrO的催化剂沉积在预先涂有混合La_2O_3-Nd_2O_3的载体上,在OCM工艺中表现出最佳性能。

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