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The Effect of Strontium Content on the Activity and Selectivity of Sr-Doped La2O3 Catalysts in Oxidative Coupling of Methane
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-09-16 , DOI: 10.1016/j.apcata.2020.117827
Robert C. Schucker , Katarzyna J. Derrickson , Azim K. Ali , Nathan J. Caton

Thirty-five doped and undoped rare earth oxide catalysts were synthesized and tested under identical conditions for the oxidative coupling of methane. While La2O3 was found to be the most active, La2O3 doped with Sr was found to be the most selective. High resolution low energy ion scattering (HR-LEIS) showed that doping with Sr above 2 mole % led to migration of Sr to the surface of the catalyst producing surface (Sr/La) ratios of 2.7 – 4.4 from bulk (Sr/La) ratios of 0.053 and 0.13, respectively. Operando Raman analysis run under OCM conditions identified La2O3 and SrCO3 as the predominant lanthanum and strontium phases during reaction. A bilayer structure comprising a thermally stable Sr-doped La2O3 base covered with a mostly amorphous Sr phase containing SrCO3, SrO and SrO2 was proposed. Selectivity to C2+ for this structure increased with surface Sr content; and SrO2 is believed to be responsible for this effect.



中文翻译:

锶含量对甲烷氧化偶联Sr掺杂La 2 O 3催化剂活性和选择性的影响

合成了35种掺杂和未掺杂的稀土氧化物催化剂,并在相同条件下对甲烷的氧化偶联进行了测试。虽然发现La 2 O 3活性最高,但发现掺杂Sr的La 2 O 3最具选择性。高分辨率低能离子散射(HR-LEIS)表明,当Sr的掺杂量大于2摩尔%时,Sr迁移至催化剂表面的生成量(Sr / La)从体积比(Sr / La)为2.7 – 4.4。比分别为0.053和0.13。在OCM条件下进行的Operando拉曼分析确定了La 2 O 3和SrCO 3作为反应过程中主要的镧和锶相。提出了一种双层结构,该双层结构包括热稳定的掺杂有Sr的La 2 O 3基层,该基层覆盖有大部分为非晶态的Sr相,其中含有SrCO 3,SrO和SrO 2。该结构对C 2 +的选择性随表面Sr含量的增加而增加。SrO 2被认为是造成这种效应的原因。

更新日期:2020-09-29
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