Evolution of reaction mechanism in the catalytic combustion of ammonia on copper-cerium mixed oxide

doi:10.1016/j.jcat.2023.06.006

CORC > 力学研究所 > 中国科学院力学研究所 > 高温气体动力学国家重点实验室

	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
刊名	JOURNAL OF CATALYSIS
	2023-09
卷号	425 页码:20-31
关键词	Catalytic combustion Ammonia CuO-CeO2 Reaction mechanism High concentration
ISSN号	0021-9517
DOI	10.1016/j.jcat.2023.06.006
英文摘要	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.
分类号	一类
WOS研究方向	Chemistry, Physical ; Engineering, Chemical
语种	英语
WOS记录号	WOS:001018622600001
资助机构	National Natural Science Foundation of China [52176142]
其他责任者	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.
内容类型	期刊论文
源URL	[http://dspace.imech.ac.cn/handle/311007/92394]
专题	力学研究所_高温气体动力学国家重点实验室
作者单位	1.{Zhao Yang, Zhang Chenhang, Dou Baojuan} Tianjin Univ Sci & Technol Coll Marine & Environm Sci Tianjin 30022 Peoples R China 2.{Liu Huan, Wang Zibing} North China Univ Sci & Technol Tangshan 063210 Hebei Peoples R China 3.{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
推荐引用方式 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.
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.