Alkali Metal-Promoted LaxSr2-xFeO4-delta Redox Catalysts for Chemical Looping Oxidative Dehydrogenation of Ethane
文献类型：期刊论文
| 作者 | Gao, Yunfei2; Haeri, Farrah2; He, Fang1 ; Li, Fanxing2
|
| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2018-03-01 |
| 卷号 | 8期号:3页码:1757-1766 |
| 关键词 | oxidative dehydrogenation chemical looping redox catalyst core-shell perovskite alkali promotion |
| ISSN号 | 2155-5435 |
| DOI | 10.1021/acscatal.7b03928 |
| 通讯作者 | Li, Fanxing(fli5@ncsu.edu) |
| 英文摘要 | Chemical looping oxidative dehydrogenation (CL-ODH) represents a redox approach to convert ethane into ethylene under an autothermal scheme. Instead of using gaseous oxygen, CL-ODH utilizes lattice oxygen in transition metal oxides, which acts as an oxygen carrier or redox catalyst, to facilitate the ODH reaction. The oxygen-deprived redox catalyst is subsequently regenerated with air and releases heat. The current study investigated alkali metal (Li, Na, and/or K)-promoted LaxSr2-x,FeO4-delta (LaSrFe) as redox catalysts for CL-ODH of ethane. While unpromoted LaSrFe exhibited poor ethylene selectivity, addition of Na or K promoter achieved up to 61% ethane conversion and 68% ethylene selectivity at 700 degrees C. The promotional effect of K on LaSrFe was characterized using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), low-energy ion scattering spectroscopy (LEIS), transmission electron microscopy (TEM), O-2-temperature-programmed desorption (TPD), H-2-temperature-programmed reduction (TPR), and O-18(2) surface exchange. XPS and XRD showed that K incorporates into the mixed-oxide structure at low loading levels (e.g., 0.1K-LaSrFe), whereas the surface of LaSrFe was enriched with K cation at high loading levels. LEIS indicates that the outermost surface layer was covered by potassium oxide. This surface layer was characterized to be amorphous under TEM. It was further determined that the surface layer increased the resistance for O2- diffusion from the bulk and its subsequent evolution into electrophilic oxygen species on the surface. As such, nonselective oxidation of ethane is inhibited. The synergistic effect of copromoting LaSrFe with Li and K was also investigated. Li and K copromotion improved the redox catalyst performance to 86% ethylene selectivity and 60% ethane conversion while maintaining an oxygen capacity of ca. 0.65 wt %, making it a promising candidate for CL-ODH. |
| WOS关键词 | METHANE PARTIAL OXIDATION ; CHLORIDE CATALYSTS ; OXIDE CATALYSTS ; LIGHT ALKANES ; OXYGEN ; POTASSIUM ; ETHYLENE ; PROPANE ; SCHEME ; KINETICS |
| 资助项目 | U.S. National Science Foundation[CBET-1604605] ; Kenan Institute for Engineering, Technology, and Science at NC State University ; State of North Carolina ; National Science Foundation |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000426804100018 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | U.S. National Science Foundation ; Kenan Institute for Engineering, Technology, and Science at NC State University ; State of North Carolina ; National Science Foundation |
| 源URL | [http://ir.giec.ac.cn/handle/344007/23284]  |
| 专题 | 中国科学院广州能源研究所 |
| 通讯作者 | Li, Fanxing |
| 作者单位 | 1.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Guangdong, Peoples R China 2.North Carolina State Univ, Dept Chem & Biomol Engn, 911 Partners Way, Raleigh, NC 27695 USA |
| 推荐引用方式 GB/T 7714 | Gao, Yunfei,Haeri, Farrah,He, Fang,et al. Alkali Metal-Promoted LaxSr2-xFeO4-delta Redox Catalysts for Chemical Looping Oxidative Dehydrogenation of Ethane[J]. ACS CATALYSIS,2018,8(3):1757-1766. |
| APA | Gao, Yunfei,Haeri, Farrah,He, Fang,&Li, Fanxing.(2018).Alkali Metal-Promoted LaxSr2-xFeO4-delta Redox Catalysts for Chemical Looping Oxidative Dehydrogenation of Ethane.ACS CATALYSIS,8(3),1757-1766. |
| MLA | Gao, Yunfei,et al."Alkali Metal-Promoted LaxSr2-xFeO4-delta Redox Catalysts for Chemical Looping Oxidative Dehydrogenation of Ethane".ACS CATALYSIS 8.3(2018):1757-1766. |
入库方式： OAI收割
来源：广州能源研究所
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