Mn-based catalysts supported on γ-Al2O3, TiO2 and MCM-41: a comparison for low-temperature NO oxidation with low ratio of O3/NO

被引:13
作者
Liu, Lijun [1 ]
Shen, Boxiong [1 ,2 ]
Si, Meng [1 ]
Yuan, Peng [1 ]
Lu, Fengju [1 ]
Gao, Hongpei [3 ]
Yao, Yan [4 ]
Liang, Cai [5 ]
Xu, Hongjie [6 ]
机构
[1] Hebei Univ Technol, Sch Energy & Environm Engn, Tianjin, Peoples R China
[2] Hebei Univ Technol, Sch Chem Engn, Tianjin, Peoples R China
[3] Clean Energy Technol Res Inst Co Ltd, China Huaneng Grp, Beijing, Peoples R China
[4] Suzhou TPRI Energy & Environm Technol Co Ltd, Suzhou, Peoples R China
[5] Chengdu Dongfang KWH Environm Protect Catalysts C, Chengdu, Peoples R China
[6] Xian Thermal Engn Inst, Xian, Peoples R China
关键词
MANGANESE OXIDE CATALYSTS; IN-SITU DRIFTS; DEEP OXIDATION; MIXED OXIDES; NITRIC-OXIDE; BENZENE OXIDATION; GASEOUS OZONE; PERFORMANCE; EFFICIENT; REDUCTION;
D O I
10.1039/d1ra01820e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Mn-Based catalysts supported on gamma-Al2O3, TiO2 and MCM-41 synthesized by an impregnation method were compared to evaluate their NO catalytic oxidation performance with low ratio O-3/NO at low temperature (80-200 degrees C). Activity tests showed that the participation of O-3 remarkably promoted the NO oxidation. The catalytic oxidation performance of the three catalysts decreased in the following order: Mn/gamma-Al2O3 > Mn/TiO2 > Mn/MCM-41, indicating that Mn/gamma-Al2O3 exhibited the best catalytic activity. In addition, there was a clear synergistic effect between Mn/gamma-Al2O3 and O-3, followed by Mn/TiO2 and O-3. The characterization results of XRD, EDS mapping, BET, H-2-TPR, XPS and TG showed that Mn/gamma-Al2O3 had good manganese dispersion, excellent redox properties, appropriate amounts of coexisting Mn3+ and Mn4+ and abundant chemically adsorbed oxygen, which ensured its good performance. In situ DRIFTS demonstrated the NO adsorption performance on the catalyst surface. As revealed by in situ DRIFTS experiments, the chemically adsorbed oxygen, mainly from the decomposition of O-3, greatly promoted the NO adsorption and the formation of nitrates. The Mn-based catalysts showed stronger adsorption strength than the corresponding pure supports. Due to the abundant adsorption sites provided by pure gamma-Al2O3, under the interaction of Mn and gamma-Al2O3, the Mn/gamma-Al2O3 catalyst exhibited the strongest NO adsorption performance among the three catalysts and produced lots of monodentate nitrates (-O-NO2) and bidentate nitrates (-O2NO), which were the vital intermediate species for NO2 formation. Moreover, the NO-TPD studies also demonstrated that Mn/gamma-Al2O3 showed the best NO desorption performance among the three catalysts. The good NO adsorption and desorption characteristics of Mn/gamma-Al2O3 improved its high catalytic activity. In addition, the activity test results also suggested that Mn/gamma-Al2O3 exhibited good SO2 tolerance.
引用
收藏
页码:18945 / 18959
页数:15
相关论文
共 81 条
[1]   The formation of 3D spherical Cr-Ce mixed oxides with roughness surface and their enhanced low-temperature NO oxidation [J].
Cai, Wei ;
Zhao, Yunxia ;
Chen, Mindong ;
Jiang, Xiaoming ;
Wang, Hu ;
Ou, Man ;
Wan, Shipeng ;
Zhong, Qin .
CHEMICAL ENGINEERING JOURNAL, 2018, 333 :414-422
[2]   High catalytic activity of Mn-based catalyst in NO oxidation at low temperature and over a wide temperature span [J].
Chen, Hu ;
Wang, Ying ;
Lyu, Yong-Kang .
MOLECULAR CATALYSIS, 2018, 454 :21-29
[3]   The catalytic performance of Mn/TiWOx catalyst for selective catalytic reduction of NOx with NH3 [J].
Chen, Qi-lin ;
Guo, Rui-tang ;
Wang, Qing-shan ;
Pan, Wei-guo ;
Wang, Wen-huan ;
Yang, Ning-zhi ;
Lu, Chen-zi ;
Wang, Shu-xian .
FUEL, 2016, 181 :852-858
[4]   Ce-Fe-Mn ternary mixed-oxide catalysts for catalytic decomposition of ozone at ambient temperatures [J].
Chen, Xiao ;
Zhao, Zhenglong ;
Liu, Shuo ;
Huang, Jinxing ;
Xie, Jing ;
Zhou, Ying ;
Pan, Zhiyan ;
Lu, Hanfeng .
JOURNAL OF RARE EARTHS, 2020, 38 (02) :175-181
[5]   Visible-light-driven deep oxidation of NO over Fe doped TiO2 catalyst: Synergic effect of Fe and oxygen vacancies [J].
Cheng, Gang ;
Liu, Xin ;
Song, Xinjie ;
Chen, Xun ;
Dai, Wenxin ;
Yuan, Rusheng ;
Fu, Xianzhi .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 277
[6]   Development of iron modified MCM-41 as promising nano-composites with specific magnetic behavior [J].
Cuello, Natalia I. ;
Elias, Veronica R. ;
Rodriguez Torres, Claudia E. ;
Crivello, Monica E. ;
Oliva, Marcos I. ;
Eimer, Griselda A. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2015, 203 :106-115
[7]   NO oxidation over Fe-based catalysts supported on montmorillonite K10, γ-alumina and ZSM-5 with gas-phase H2O2 [J].
Cui, Rongji ;
Ma, Suxia ;
Wang, Jie ;
Sun, Shujun .
CHEMOSPHERE, 2019, 234 :302-309
[8]   Post plasma-catalysis for total oxidation of trichloroethylene over Ce-Mn based oxides synthesized by a modified "redox-precipitation route" [J].
Dinh, M. T. Nguyen ;
Giraudon, J. -M. ;
Vandenbroucke, A. M. ;
Morent, R. ;
De Geyter, N. ;
Lamonier, J. -F. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 172 :65-72
[9]   Oxidation behavior of cyclohexane on alumina-supported manganese oxides with ozone [J].
Einaga, H ;
Futamura, S .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 60 (1-2) :49-55
[10]   Catalytic properties of copper-manganese mixed oxides supported on SiO2 for benzene oxidation with ozone [J].
Einaga, Hisahiro ;
Maeda, Nanako ;
Yamamoto, Shintaro ;
Teraoka, Yasutake .
CATALYSIS TODAY, 2015, 245 :22-27