Distinct structure-activity relationship and reaction mechanism over CuO/ CeO<sub>2</sub> catalysts for NH3 self-sustained combustion

doi:10.1016/j.proci.2024.105647

	Distinct structure-activity relationship and reaction mechanism over CuO/ CeO₂ catalysts for NH3 self-sustained combustion
	Kang RN(康润宁)1 ; Zhang CH(张晨航)1,2; Zhang ZR(张梓睿)1,3; Bin F(宾峰)1,3 ; Yi XK(衣晓坤)1,4; Huang JQ(黄俊钦)1,3; Wei XL(魏小林)1,3
通讯作者	Bin, Feng([email protected]) ; Wei, Xiaolin([email protected])
发表期刊	PROCEEDINGS OF THE COMBUSTION INSTITUTE
	2024
卷号	40 期号:1-4 页码:7
ISSN	1540-7489
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.
关键词	Ammonia CuO/CeO2 Self-sustained combustion Structure-activity relationship Reaction mechanism
DOI	10.1016/j.proci.2024.105647
收录类别	SCI ; EI
语种	英语
WOS记录号	WOS:001297553800001
关键词[WOS]	OXIDATION ; AMMONIA
WOS研究方向	Thermodynamics ; Energy & Fuels ; Engineering
WOS类目	Thermodynamics ; Energy & Fuels ; Engineering, Chemical ; Engineering, Mechanical
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]
项目资助者	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
论文分区	一类
力学所作者排名	1
RpAuthor	Bin, Feng ; Wei, Xiaolin
引用统计	被引频次：2[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://dspace.imech.ac.cn/handle/311007/96382
专题	高温气体动力学国家重点实验室
作者单位	1.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China; 2.Beijing Univ Technol, Fac Environm & Life, Key Lab Beijing Reg Air Pollut Control, Beijing 100124, Peoples R China; 3.Univ Chinese Acad Sci, Sch Engn Sci, Beijing 100049, Peoples R China; 4.Tianjin Univ Sci & Technol, Coll Marine & Environm Sci, Tianjin 300457, Peoples R China
推荐引用方式 GB/T 7714	Kang RN,Zhang CH,Zhang ZR,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.Rp_Au:Bin, Feng, Wei, Xiaolin
APA	康润宁.,张晨航.,张梓睿.,宾峰.,衣晓坤.,...&魏小林.(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	康润宁,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.