Strikingly distinctive NH3-SCR behavior over Cu-SSZ-13 in the presence of NO2
文献类型：期刊论文
| 作者 | Shan, Yulong; He, Guangzhi ; Du, Jinpeng; Sun, Yu; Liu, Zhongqi; Fu, Yu; Liu, Fudong; Shi, Xiaoyan; Yu, Yunbo; He, Hong
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| 刊名 | NATURE COMMUNICATIONS
 |
| 出版日期 | 2022-08-08 |
| 卷号 | 13期号:1页码:4606 |
| 关键词 | SELECTIVE CATALYTIC-REDUCTION HYDROTHERMAL STABILITY SSZ-13 ZEOLITE SITES TRANSIENT OXIDATION KINETICS AMMONIA FRESH IONS |
| 英文摘要 | Cu-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. |
| 源URL | [https://ir.rcees.ac.cn/handle/311016/47428]  |
| 专题 | 生态环境研究中心_大气污染控制中心 |
| 作者单位 | 1.Chinese Acad Sci, Key Lab Urban Pollutant Convers, Inst Urban Environm, Xiamen 361021, Peoples R China 2.Univ Cent Florida, Dept Civil Environm & Construct Engn, Catalysis Cluster Renewable Energy & C 3.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China 4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 5.Chinese Acad Sci, Ctr Excellence Reg Atmospher Environm, Inst Urban Environm, Xiamen 361021, Peoples R China |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：生态环境研究中心
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