In Situ DRIFTs Investigation of the Low-Temperature Reaction Mechanism over Mn-Doped Co3O4 for the Selective Catalytic Reduction of NOx with NH3

被引:262
作者
Hu, Hang [1 ]
Cai, Sixiang [1 ]
Li, Hongrui [1 ]
Huang, Lei [1 ]
Shi, Liyi [1 ,2 ]
Zhang, Dengsong [1 ]
机构
[1] Shanghai Univ, Res Ctr Nano Sci & Technol, Shanghai 200444, Peoples R China
[2] Shanghai Univ, Dept Chem, Shanghai 200444, Peoples R China
基金
中国国家自然科学基金;
关键词
MIXED-OXIDE CATALYST; NITROGEN-OXIDES; ACTIVE OXYGEN; NITRIC-OXIDE; OXIDATION; PERFORMANCE; AMMONIA; FE; CO; SCR;
D O I
10.1021/acs.jpcc.5b06057
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
The Co3O4 and Mn-doped Co3O4 nanopartide were synthesized by a co-precipitation method and used as selective catalytic reduction of NO with NH3 (NH3-SCR) catalysts. After the doping of manganese oxides, the NH3-SCR activity of Mn0.05Co0.95Ox catalyst is greatly enhanced. The NO oxidation ability of two catalysts is compared, and the X-ray diffraction results demonstrate that Mn has been successfully doped into the lattice of Co3O4. The X-ray photoelectron spectroscopy and temperature-programmed reduction with H-2 results confirmed that there is a strong interaction between Mn and Co in the Mn0.05Co0.95Ox, catalyst. Their adsorption and desorption properties were characterized by temperature-programmed desorption with NH3 or NO + O-2 and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs). These results indicated that the doping of manganese could provide more acid sites on the catalysts, and bidentate nitrates species originated from NOx adsorption are obviously activated on the Mn0.05Co0.95Ox catalyst surface. Moreover, the transient reaction studied by in situ DRIFTs found that the "fast SCR" reaction participated by gaseous NO2 and the standard SCR reaction participated by bidentate nitrates contribute to the low-temperature SCR activity.
引用
收藏
页码:22924 / 22933
页数:10
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