Experimental and Theoretical Investigation of Mesoporous MnO2 Nanosheets with Oxygen Vacancies for High-Efficiency Catalytic DeNOx

被引:137
作者
Liu, Jia [1 ]
Wei, Yajuan [1 ,2 ]
Li, Pei-Zhou [1 ]
Zhang, Peipei [2 ]
Su, Wei [4 ]
Sun, Yan [2 ]
Zou, Ruqiang [3 ]
Zhao, Yanli [1 ]
机构
[1] Nanyang Technol Univ, Sch Phys & Math Sci, Div Chem & Biol Chem, 21 Nanyang Link, Singapore 637371, Singapore
[2] Tianjin Univ, Sch Sci, Dept Chem, High Pressure Adsorpt Lab, Tianjin 300350, Peoples R China
[3] Peking Univ, Dept Mat Sci & Engn, Coll Engn, Beijing Key Lab Theory & Technol Adv Battery Mat, Beijing 100871, Peoples R China
[4] Tianjin Univ, Tianjin Key Lab Membrane & Desalinat Technol, Sch Chem Engn & Technol, Tianjin 300350, Peoples R China
基金
中国国家自然科学基金;
关键词
DeNO(x); density functional theory; diffuse reflectance infrared Fourier transform; mesoporous MnO2; selective catalytic reduction; LOW-TEMPERATURE SCR; MANGANESE OXIDE CATALYSTS; NO REDUCTION; MNOX/TIO2; CATALYSTS; N2O DECOMPOSITION; SUPERIOR CATALYST; MN/TIO2; CARBON NANOTUBES; DOPED MN/TIO2; NITRIC-OXIDE;
D O I
10.1021/acscatal.8b00267
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
A solvent-free synthetic method was employed for the construction of mesoporous alpha-MnO2 nanosheets. Benefiting from a solid interface reaction, the obtained MnO2 nanosheets with large oxygen vacancies exhibit a high surface area of up to 339 m(2)/g and a mesopore size of 4 nm. The MnO2 nanosheets as a catalyst were applied in NH3-assisted selective catalytic reduction (NH3-SCR) of DeNO(x) at a relatively low temperature range. The conversion efficiency could reach 100% under a gas hourly space velocity (GHSV) of 700000 h(-1) at 100 degrees C. To gain insight into the mechanism about NH3-SCR of nitric oxide on the MnO2 nanosheets, temperature-programmed desorption of NH3, a density functional theory study, and in situ diffuse reflectance infrared Fourier transform spectra were carried out, revealing the cooperative effect of catalytic sites on the reduction of nitric oxide. This work provides a strategy for the facile preparation of porous catalysts in low-temperature DeNO(x).
引用
收藏
页码:3865 / 3874
页数:19
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