Distinct structure-activity relationship and reaction mechanism over CuO/ CeO2 catalysts for NH3 self-sustained combustion
文献类型：期刊论文
| 作者 | Kang, Running4 ; Zhang, Chenhang3,4; Zhang, Zirui2,4; Bin, Feng2,4; Yi, Xiaokun1,4; Huang, Junqin2,4; Wei, Xiaolin2,4; Wei XL(魏小林); Bin F(宾峰); Kang RN(康润宁)
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| 刊名 | PROCEEDINGS OF THE COMBUSTION INSTITUTE
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| 出版日期 | 2024 |
| 卷号 | 40期号:1-4页码:7 |
| 关键词 | Ammonia CuO/CeO2 Self-sustained combustion Structure-activity relationship Reaction mechanism |
| ISSN号 | 1540-7489 |
| DOI | 10.1016/j.proci.2024.105647 |
| 通讯作者 | Bin, Feng(binfeng@imech.ac.cn) ; Wei, Xiaolin(xlwei@imech.ac.cn) |
| 英文摘要 | The catalytic combustion of NH3 to produce nitrogen (N-2) and water (H2O) is a promising method to solve high ignition temperature with more NOx production and poor combustion stability in the carbon-free fuel utilization of NH3. This study focuses on distinct structure-activity relationship over CuO/CeO2 series catalysts and reaction mechanism for catalytic NH3 combustion. Cu/Ce-Sphere, Cu/Ce-Rod, and Cu/Ce-Octahedron catalysts were synthesized through an impregnation method by using different CeO2 carriers (nano sphere (S), rod (R) and octahedron (O)). The activity for NH3 combustion followed an order of Cu/Ce-S > Cu/Ce-R > Cu/Ce-O > Ce-S. The better activity of Cu/Ce-S is attributed to the strong interaction between CuO and Ce-S (111 and 220 planes) at the interface of oxide phases. This interaction is indicative of a higher specific surface area (SSA) to promote CuOx dispersion, facilitating the adsorption of ammonia. Additionally, more Cu-O-x-Ce solid solution with oxygen vacancies enhances the formation and mobility of active oxygen species. The Cu/Ce-S showed a low NH3 lean-combustion limits of 7.6 % NH3 to keep self-sustained combustion, and realized a high NH3 conversion (similar to 100 %) and effective N-2 yield (similar to 98.0 %) with low NOx formation over 360 min. The reaction pathways for NH3 combustion over Cu/Ce-S were revealed by the NH3-TPD/TPR-mass spectrometer, isotopic (O-18(2)) transient exchange experiment and in situ infrared transmission spectroscopy (IR). The Mars-van-Krevelen (M-K) mechanism plays a crucial contribution of adsorbed NHx by ammonia dehydrogenation route to react with active lattice oxygen, and to produce N-2 and H2O. Additionally, the subordinate contribution of Langmuir-Hinshelwood (L-H) mechanism refers the reaction of adsorbed NHx species and chemisorbed oxygen or adsorbed HNO through oxidation route. These results demonstrate the viability of environmentally friendly catalytic combustors for ammonia fuel in the future, and also advance the understanding of reaction mechanism for catalytic ammonia combustion. |
| WOS关键词 | OXIDATION ; AMMONIA |
| 资助项目 | National Natural Science Foundation of China[52176142] ; China National Postdoctoral Program for Innovative Talents[BX20230380] ; Youth Fund of the State Key Laboratory of High Temperature Gas Dynamics[2023QN07] |
| WOS研究方向 | Thermodynamics ; Energy & Fuels ; Engineering |
| 语种 | 英语 |
| WOS记录号 | WOS:001297553800001 |
| 资助机构 | National Natural Science Foundation of China ; China National Postdoctoral Program for Innovative Talents ; Youth Fund of the State Key Laboratory of High Temperature Gas Dynamics |
| 源URL | [http://dspace.imech.ac.cn/handle/311007/96381]  |
| 专题 | 力学研究所_高温气体动力学国家重点实验室 |
| 通讯作者 | Bin, Feng; Wei, Xiaolin |
| 作者单位 | 1.Tianjin Univ Sci & Technol, Coll Marine & Environm Sci, Tianjin 300457, Peoples R China 2.Univ Chinese Acad Sci, Sch Engn Sci, Beijing 100049, Peoples R China 3.Beijing Univ Technol, Fac Environm & Life, Key Lab Beijing Reg Air Pollut Control, Beijing 100124, Peoples R China 4.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China |
| 推荐引用方式 GB/T 7714 | Kang, Running,Zhang, Chenhang,Zhang, Zirui,et al. Distinct structure-activity relationship and reaction mechanism over CuO/ CeO2 catalysts for NH3 self-sustained combustion[J]. PROCEEDINGS OF THE COMBUSTION INSTITUTE,2024,40(1-4):7. |
| APA | Kang, Running.,Zhang, Chenhang.,Zhang, Zirui.,Bin, Feng.,Yi, Xiaokun.,...&康润宁.(2024).Distinct structure-activity relationship and reaction mechanism over CuO/ CeO2 catalysts for NH3 self-sustained combustion.PROCEEDINGS OF THE COMBUSTION INSTITUTE,40(1-4),7. |
| MLA | Kang, Running,et al."Distinct structure-activity relationship and reaction mechanism over CuO/ CeO2 catalysts for NH3 self-sustained combustion".PROCEEDINGS OF THE COMBUSTION INSTITUTE 40.1-4(2024):7. |
入库方式： OAI收割
来源：力学研究所
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