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Strikingly distinctive NH3-SCR behavior over Cu-SSZ-13 in the presence of NO2
Shan, Yulong; He, Guangzhi; Du, Jinpeng; Sun, Yu; Liu, Zhongqi; Fu, Yu; Liu, Fudong; Shi, Xiaoyan; Yu, Yunbo; He, Hong
2022-08-08
Source PublicationNATURE COMMUNICATIONS
Volume13Issue:1Pages:4606
AbstractCu-SSZ-13 zeolites are highly active for standard NH3-SCR, but their activity is unexpectedly inhibited in the presence of NO2. This work demonstrates that strong oxidation by NO2 forces Cu ions to exist mainly as Cu-II species with low mobility, which is responsible for this distinctive behavior. Commercial Cu-exchanged small-pore SSZ-13 (Cu-SSZ-13) zeolite catalysts are highly active for the standard selective catalytic reduction (SCR) of NO with NH3. However, their activity is unexpectedly inhibited in the presence of NO2 at low temperatures. This is strikingly distinct from the NO2-accelerated NOx conversion over other typical SCR catalyst systems. Here, we combine kinetic experiments, in situ X-ray absorption spectroscopy, and density functional theory (DFT) calculations to obtain direct evidence that under reaction conditions, strong oxidation by NO2 forces Cu ions to exist mainly as Cu-II species (fw-Cu2+ and NH3-solvated Cu-II with high CNs), which impedes the mobility of Cu species. The SCR reaction occurring at these Cu-II sites with weak mobility shows a higher energy barrier than that of the standard SCR reaction on dynamic binuclear sites. Moreover, the NO2-involved SCR reaction tends to occur at the Bronsted acid sites (BASs) rather than the Cu-II sites. This work clearly explains the strikingly distinctive selective catalytic behavior in this zeolite system.
Department大气环境与污染控制实验室 ; 大气环境与污染控制实验室
KeywordSELECTIVE CATALYTIC-REDUCTION HYDROTHERMAL STABILITY SSZ-13 ZEOLITE SITES TRANSIENT OXIDATION KINETICS AMMONIA FRESH IONS
Document Type期刊论文
Identifierhttps://ir.rcees.ac.cn/handle/311016/47428
Collection大气环境与污染控制实验室
Affiliation1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China
2.Chinese Acad Sci, Ctr Excellence Reg Atmospher Environm, Inst Urban Environm, Xiamen 361021, Peoples R China
3.Chinese Acad Sci, Key Lab Urban Pollutant Convers, Inst Urban Environm, Xiamen 361021, Peoples R China
4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
5.Univ Cent Florida, Dept Civil Environm & Construct Engn, Catalysis Cluster Renewable Energy & C
Recommended Citation
GB/T 7714
Shan, Yulong,He, Guangzhi,Du, Jinpeng,et al. Strikingly distinctive NH3-SCR behavior over Cu-SSZ-13 in the presence of NO2[J]. NATURE COMMUNICATIONS,2022,13(1):4606.
APA Shan, Yulong.,He, Guangzhi.,Du, Jinpeng.,Sun, Yu.,Liu, Zhongqi.,...&He, Hong.(2022).Strikingly distinctive NH3-SCR behavior over Cu-SSZ-13 in the presence of NO2.NATURE COMMUNICATIONS,13(1),4606.
MLA Shan, Yulong,et al."Strikingly distinctive NH3-SCR behavior over Cu-SSZ-13 in the presence of NO2".NATURE COMMUNICATIONS 13.1(2022):4606.
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