| Ca,Sr共掺杂铈氧化物及其在甲烷氧化偶联反应中的应用 |
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| 引用本文： | 杨艳玲,董玲玉,夏文生,万惠霖.Ca,Sr共掺杂铈氧化物及其在甲烷氧化偶联反应中的应用[J].高等学校化学学报,2016(12):2206-2214. |
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| 作者姓名： | 杨艳玲 董玲玉 夏文生 万惠霖 |
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| 作者单位： | 厦门大学化学化工学院，固体表面物理化学国家重点实验室，醇醚酯化工清洁生产国家工程实验室，福建省理论计算化学重点实验室，厦门361005 |
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| 基金项目： | 国家自然科学基金(批准号21373169)，教育部“长江学者和创新团队发展计划”项目(批准号IRT1036)资助．? Supported by the National Natural Science Foundation of China(21373169)，the Program for Changjiang Scholars and Innovative Research Team in the University， China( No． IRT1036)． |
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| 摘 要： | 采用柠檬酸法制备了Ca,Sr共掺杂的CeO_2催化剂,发现共掺杂催化剂较单掺杂或未掺杂催化剂呈现出更好的催化甲烷氧化偶联(OCM)反应性能.通过表征可知,Ca,Sr共掺杂催化剂的物相为CeO_2和SrCO_3,Ca高度分散或掺杂于CeO_2之中;CeO_2的粒径明显变小;表面呈中等程度碱性;Ce基催化剂上的亲电氧物种数量随着碱土金属的掺杂而增大,亲电氧物种与晶格氧摩尔比(O_2-2+O-2)/O-2的大小顺序(CeSrCaCe SrCeO_2)与C2选择性一致;且SrCO_3相的存在有助于Ce基氧化物催化甲烷氧化偶联反应(OCM)性能的改善.
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| 关 键 词： | 碱土金属 掺杂 CeO2 碳酸盐 甲烷氧化偶联 |
Ca,Sr co-Doped Ceria and Its Application in Oxidative Coupling of Methane |
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| Abstract: | The Ca and Sr co?doped ceria catalysts were synthesized with a citric acid method and their performances in oxidative coupling of methane ( OCM ) were significantly enhanced when compared with the single or none doped ceria catalysts. By X?ray diffraction(XRD), CO2 temperature programmed desorption ( CO2?TPD) , O2 temperature programmed desorption ( O2?TPD ) , X?ray photoelectron spectroscopy ( XPS ) characterizations, we found that the Ca and Sr co?doped catalysts were consisted of the phases CeO2 and SrCO3 , along with Ca highly dispersed or doped in ceria. They exhibited the decreased size of ceria particles and the medium basicity. The number of electrophilic oxygen species and the ratio of electrophilic oxygen species to lattice oxygen species on the catalyst surfaces were changed in the order of CeSrCa>CeSr>CeO2 , corresponding to the C2 selectivity in OCM. In addition, the presence of SrCO3 was beneficial to improve on catalytic performances of OCM over Ce?based oxide catalysts. |
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| Keywords: | Alkali earth Dope Ceria Carbonate Oxidative coupling of methane |
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