Reaction Pathways of the Selective Catalytic Reduction of NO with NH3 on the alpha-Fe2O3(012) Surface: a Combined Experimental and DFT Study
文献类型：期刊论文
| 作者 | Gao, Meng; He, Guangzhi; Zhang, Wenshuo; Du, Jinpeng ; He, Hong
|
| 刊名 | ENVIRONMENTAL SCIENCE & TECHNOLOGY
 |
| 出版日期 | 2021-08-17 |
| 卷号 | 55期号:16页码:10967-10974 |
| ISSN号 | 0013-936X |
| 关键词 | NH3-SCR reaction mechanism Fe2O3-based catalysts DFT calculation in situ DRIFTS |
| 英文摘要 | Fe2O3-based catalysts have promising potential in the selective catalytic reduction (SCR) of NO with NH3 with the advantages of environmental friendliness, excellent medium-high SCR activity, good N-2 selectivity, and high SO2 tolerance. However, the NH3-SCR mechanism over Fe2O3 -based catalysts remains highly uncertain and controversial due to the complex nature of the SCR reaction. Herein, the NH3-SCR reaction pathways over the alpha-Fe2O3 (012) surface are elucidated at the atomic level by density functional theory calculations and experimental measurements. We demonstrate that, different from the NH3 activation mechanism in numerous SCR catalytic systems, the reaction tends to follow the NO activation mechanism, in which NO activated at Fe sites reacts with NH3 to form a NH2NO intermediate and further decomposes into N-2 and H2O, in synchronization with the formation of a surface OH group. Subsequently, the catalyst is regenerated by an O-2-assisted surface- dehydrogenation process. The activation of NO as well as the formation of the NH2 NO intermediate is the rate-determining step of the complete SCR cycle. This study enhances the atomic-level understanding toward the NH3-SCR reaction and provides insights for the development of Fe2O3-based SCR catalysts. |
| WOS研究方向 | Engineering, Environmental ; Environmental Sciences |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/46066]  |
| 专题 | 生态环境研究中心_水污染控制实验室 |
| 作者单位 | 1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 2.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China 3.Chinese Acad Sci, Ctr Excellence Reg Atmospher Environm, Inst Urban Environm, Xiamen 361021, Peoples R China |
| 推荐引用方式 GB/T 7714 | Gao, Meng,He, Guangzhi,Zhang, Wenshuo,et al. Reaction Pathways of the Selective Catalytic Reduction of NO with NH3 on the alpha-Fe2O3(012) Surface: a Combined Experimental and DFT Study[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2021,55(16):10967-10974. |
| APA | Gao, Meng,He, Guangzhi,Zhang, Wenshuo,Du, Jinpeng,&He, Hong.(2021).Reaction Pathways of the Selective Catalytic Reduction of NO with NH3 on the alpha-Fe2O3(012) Surface: a Combined Experimental and DFT Study.ENVIRONMENTAL SCIENCE & TECHNOLOGY,55(16),10967-10974. |
| MLA | Gao, Meng,et al."Reaction Pathways of the Selective Catalytic Reduction of NO with NH3 on the alpha-Fe2O3(012) Surface: a Combined Experimental and DFT Study".ENVIRONMENTAL SCIENCE & TECHNOLOGY 55.16(2021):10967-10974. |
入库方式： OAI收割
来源：生态环境研究中心
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