| Evolution of reaction mechanism in the catalytic combustion of ammonia on copper-cerium mixed oxide | |
Liu, Huan; Zhao, Yang; Zhang, Chenhang; Wang, Zibing; Bin F(宾峰) ; Wei XL(魏小林); Dou, Baojuan
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| Source Publication | JOURNAL OF CATALYSIS
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| 2023-09 | |
| Volume | 425Pages:20-31 |
| ISSN | 0021-9517 |
| Abstract | Carbon-free hydrogen-rich ammonia (NH3) is a potential next energy generation source, where a high ignition point and high nitric oxide contents, thereby limiting further development. This study aims to investigate the mechanism evolution during the catalytic ignition process of high NH3 concentration over copper-cerium catalyst to address the demerits of flame combustion. The phase composition, elemental valence, and active species of the copper-cerium oxide (CuO-CeO2) catalyst are investigated using various characterization techniques. The results indicated that Cu species are mainly present in copper-cerium solid solutions and highly dispersed CuO clusters, providing sufficient Cu sites to adsorb NH3 and abun-dant reactive lattice oxygen. The catalytic ignition triggered a kinetic transition from low-rate to high -rate steady-state. During the induction process, the predominance of the L-H mechanism is implied by the kinetic modeling and transient experiments (low-rate induced phase). Combined with IR spec-troscopy and isotope (18O2)-transient response study, the results indicated that adsorbed NH3 reacted with surface adsorbed oxygen, simultaneously pulling out lattice oxygen to react with adsorbed NH3, confirming the coexistence of L-H and M-K mechanism over CuO-CeO2. The L-H mechanism (18O, con-tribution of adsorbed oxygen) plays a relatively dominant role in the induction stage, while the involve-ment of the M-K mechanism (16O, contribution of lattice oxygen) is significantly increased in the sustained combustion stage. At both stages, NH and NH2 served as critical species for N2 generation (i-SCR), respectively, playing an important role in N2 selectivity. Moreover, in the self-sustained combustion stage for CuO-CeO2 (14%NH3), the rapid gas diffusion and mass transfer facilitated the adsorption and activation of NH3. These results are envisaged to provide theoretical support for the handling and appli-cation of high concentrations of NH3.& COPY; 2023 Elsevier Inc. All rights reserved. |
| Keyword | Catalytic combustion Ammonia CuO-CeO2 Reaction mechanism High concentration |
| DOI | 10.1016/j.jcat.2023.06.006 |
| Indexed By | SCI ; EI |
| Language | 英语 |
| WOS ID | WOS:001018622600001 |
| WOS Research Area | Chemistry, Physical ; Engineering, Chemical |
| Funding Organization | National Natural Science Foundation of China [52176142] |
| Classification | 一类 |
| Ranking | 1 |
| Contributor | Bin, F (corresponding author), Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China. ; Dou, BJ (corresponding author), Tianjin Univ Sci & Technol, Coll Marine & Environm Sci, Tianjin 30022, Peoples R China. |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://dspace.imech.ac.cn/handle/311007/92394 |
| Collection | 高温气体动力学国家重点实验室 |
| Affiliation | 1.{Liu Huan, Zhang Chenhang, Bin Feng, Wei Xiaolin} Chinese Acad Sci Inst Mech State Key Lab High Temp Gas Dynam Beijing 100190 Peoples R China 2.{Liu Huan, Wang Zibing} North China Univ Sci & Technol Tangshan 063210 Hebei Peoples R China 3.{Zhao Yang, Zhang Chenhang, Dou Baojuan} Tianjin Univ Sci & Technol Coll Marine & Environm Sci Tianjin 30022 Peoples R China |
| Recommended Citation GB/T 7714 | Liu, Huan,Zhao, Yang,Zhang, Chenhang,et al. Evolution of reaction mechanism in the catalytic combustion of ammonia on copper-cerium mixed oxide[J]. JOURNAL OF CATALYSIS,2023,425:20-31.Rp_Au:Bin, F (corresponding author), Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China., Dou, BJ (corresponding author), Tianjin Univ Sci & Technol, Coll Marine & Environm Sci, Tianjin 30022, Peoples R China. |
| APA | Liu, Huan.,Zhao, Yang.,Zhang, Chenhang.,Wang, Zibing.,宾峰.,...&Dou, Baojuan.(2023).Evolution of reaction mechanism in the catalytic combustion of ammonia on copper-cerium mixed oxide.JOURNAL OF CATALYSIS,425,20-31. |
| MLA | Liu, Huan,et al."Evolution of reaction mechanism in the catalytic combustion of ammonia on copper-cerium mixed oxide".JOURNAL OF CATALYSIS 425(2023):20-31. |
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| Jp2023Fa158.pdf（4108KB） | 期刊论文 | 出版稿 | 开放获取 | CC BY-NC-SA | View Download | |
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