Revealing the mechanisms of NH3 adsorption and reactions in catalytic NOx reduction over Cux/CHA zeolites by in situ DRIFTS spectroscopy

被引:1
|
作者
Shen, Yali [1 ]
Wang, Zhiqiang [2 ,3 ]
Ge, Shasha [1 ]
Wang, Li [1 ]
Zhan, Wangcheng [1 ]
Dai, Qiguang [1 ]
Guo, Yanglong [1 ]
Guo, Yun [1 ]
Wang, Aiyong [1 ]
机构
[1] East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China
[2] East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China
[3] East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China
基金
中国国家自然科学基金;
关键词
NH3-SCR; Cu-SSZ-13; NH3; solvation; Intra-zeolite oxolation; REACTION-KINETICS; CU-SSZ-13; NH3-SCR; CU/SSZ-13; IONS;
D O I
10.1016/j.apcatb.2024.124094
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Adsorption and activation of NH3 on Cu-SSZ-13 were essential for NOx removal, however, their important role at the molecular level remains unclear. In this work, the Al-rich Cu/SSZ-13 (Cu-x/CHA) catalysts were synthesized by the incipient-wetness impregnation method, and the NH3-SCR performance was investigated. It is found that high Cu content promoted the formation of Z-[Cu(OH)](+) and CuOx particles, enhanced the adsorption capacity of NOx, and increased the intra-zeolite oxolation process in the Cu-x/CHA catalysts. In situ DRIFTS results showed that the Z-[Cu(OH)(NH3)(x)]+(x<3) exhibited analogous properties to B-NH4+, but it would convert to Z-[Cu(OH) (NH3)(3)](+) with increasing NH3 adsorption time and exhibit L-NH3 properties. Those findings could provide a new insight into understanding the adsorption and activation of NH3 in low-temperature reactions, as well as new ideas for improving NOx conversion during cold start.
引用
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页数:12
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