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Unraveling high-temperature mechanism of NO

文献类型：期刊论文

作者Xu, Kangwei1,2; Zhang, Wei1,2; Ye, Yue1,2; Song, Qianshi2; Zhang, Lidong3; Wang, Xiaohan1,2
刊名JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
出版日期2024-10-01
卷号12期号:5页码:11
关键词NO reduction BaO-Y2O3 High temperature MvK mechanism BaCO3
ISSN号2213-2929
DOI10.1016/j.jece.2024.114103
通讯作者Zhang, Lidong(zld@ustc.edu.cn) ; Wang, Xiaohan(wangxh@ms.giec.ac.cn)
英文摘要Understanding high-temperature mechanism of NO reduction by CO on heat-resistant metal oxides is crucial for exhaust aftertreatment systems. We employed the NO + CO light off experiment, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), density functional theory (DFT), and microkinetic study to elucidate the reaction mechanism on BaO-Y2O3 nanocatalyst. The catalytic cycle consisting of "decomposition-oxidation" mode, Mars-van Krevelen (MvK) mechanism, and Langmuir-Hinshelwood (L-H) mechanism is described by in situ DRIFTS and DFT calculations. Their reaction energies and activation barriers are then employed for the microkinetic analysis, revealing that the activity rate is temperature-dependent and aligns with the experimental result. The high-temperature reaction process is primarily governed by the MvK mechanism with rate-determining steps (RDS) of CO + O-L <-> CO2 + Ov, followed by the "decomposition-oxidation" mode. Critically, local CO32- coverage on the BaO surface can facilitate NO and CO adsorption while withstanding the elementary steps such as N2O dissociation and CO oxidation by lattice oxygen. BaCO3-Y2O3 model can be used to interpret the low-temperature reaction process with the RDS of N2O2 <-> N2O + O, but it impedes reaction kinetics at high temperatures with the rate contribution also predominantly originating from the MvK mechanism. This work provides fundamental insights into how the reaction proceed, and guide the design and optimization of catalysts that can withstand high temperature while maintaining high activity.
WOS关键词SELECTIVE CATALYTIC-REDUCTION ; DIRECT DECOMPOSITION ; DOPED CEO2 ; CO ; OXIDATION ; OXIDE ; Y2O3 ; O-2 ; MN
资助项目Special Project for Research and Development in Key Areas of Guangdong Province[2020B1111360004] ; National Natural Science Foundation of China[52206285] ; Science Fund for Distinguished Young Scholars of Anhui Province[2308085J20] ; Basic and Applied Basic Research Foundation of Guangdong Province[2024A1515011639] ; China Post-doctoral Science Foundation[2022M723161] ; China Post-doctoral Science Foundation[2023T160648]
WOS研究方向Engineering
语种英语
WOS记录号WOS:001315965200001
出版者ELSEVIER SCI LTD
资助机构Special Project for Research and Development in Key Areas of Guangdong Province ; National Natural Science Foundation of China ; Science Fund for Distinguished Young Scholars of Anhui Province ; Basic and Applied Basic Research Foundation of Guangdong Province ; China Post-doctoral Science Foundation
源URL[http://ir.giec.ac.cn/handle/344007/42921]  
专题中国科学院广州能源研究所
通讯作者Zhang, Lidong; Wang, Xiaohan
作者单位1.Univ Sci & Technol China, Sch Energy Sci & Engn, Hefei 230029, Peoples R China
2.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Peoples R China
3.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
推荐引用方式
GB/T 7714		 Xu, Kangwei,Zhang, Wei,Ye, Yue,et al. Unraveling high-temperature mechanism of NO[J]. JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING,2024,12(5):11.
APA Xu, Kangwei,Zhang, Wei,Ye, Yue,Song, Qianshi,Zhang, Lidong,&Wang, Xiaohan.(2024).Unraveling high-temperature mechanism of NO.JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING,12(5),11.
MLA Xu, Kangwei,et al."Unraveling high-temperature mechanism of NO".JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 12.5(2024):11.

入库方式： OAI收割

来源：广州能源研究所

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