Unusual positive effect of SO2 on Mn-Ce mixed-oxide catalyst for the SCR reaction of NOx with NH3

被引:135
作者
Chen, JiaYu [1 ]
Fu, Peng [1 ]
Lv, Daofei [1 ]
Chen, Yang [1 ]
Fan, Meiling [1 ]
Wu, Junliang [2 ]
Meshram, Amogh [3 ]
Mu, Bin [3 ]
Li, Xiang [4 ]
Xia, Qibin [1 ]
机构
[1] South China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510641, Peoples R China
[2] South China Univ Technol, Guangzhou Higher Educ Mega Ctr, Guangdong Prov Key Lab Atmospher Environm & Pollu, Guangzhou 510006, Peoples R China
[3] Arizona State Univ, Sch Engn Matter Transport & Energy, Tempe, AZ 85287 USA
[4] South China Univ Technol, Sch Publ Adm, Guangzhou 510640, Peoples R China
基金
中国国家自然科学基金;
关键词
Denitration catalysts; SCR; SO2; tolerance; Mn-Ce mixed oxides; LOW-TEMPERATURE SCR; MANGANESE OXIDES; MNOX/TIO2; CATALYSTS; CARBON NANOTUBES; NH3-SCR ACTIVITY; REDUCTION; OXIDATION; RESISTANCE; MECHANISM; REMOVAL;
D O I
10.1016/j.cej.2020.127071
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A high-performance denitration catalyst based on Mn-Ce mixed-oxide derived from a specific Mn/Ce pre-cursorwas fabricated by solvothermal method. It exhibited outstanding low-temperature activity, which achieved above 90% NOx conversion in the temperature of 150-310 degrees C. Remarkably, Mn-Ce mixed-oxide demonstrated a much better SO2 tolerance, in which the NOx conversion increased from 92.6% to 97.8% at 150 degrees C after introducing 200 ppm SO2. The synthesized Mn-Ce mixed-oxide has a porous structure with abundant chemisorbed oxygen spices and exposed active sites. In addition, the increased acidity and redox capacity enhanced the catalytic activity after introducing SO2. Meanwhile, the injection of SO2 separates NH3 adsorption sites from oxidation agents, inhibiting the unwanted oxidization of ammonia to nitrogen oxides. Furthermore, the reaction pathway on Mn-Ce mixed-oxide proved to be the L-H mechanism based on in situ DRIFTS. Thus, the synthesized Mn-Ce mixed oxide demonstrated an excellent denitration performance and the especially high SO2 tolerance, showing great potential for low-temperature NH3-SCR.
引用
收藏
页数:10
相关论文
共 92 条
[1]   Unified mechanistic model for Standard SCR, Fast SCR, and NO2 SCR over a copper chabazite catalyst [J].
Bendrich, M. ;
Scheuer, A. ;
Hayes, R. E. ;
Votsmeier, M. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 222 :76-87
[2]   Effect of Sn on MnOx-CeO2 catalyst for SCR of NOx by ammonia: Enhancement of activity and remarkable resistance to SO2 [J].
Chang, Huazhen ;
Li, Junhua ;
Chen, Xiaoyin ;
Ma, Lei ;
Yang, Shijian ;
Schwank, Johannes W. ;
Hao, Jiming .
CATALYSIS COMMUNICATIONS, 2012, 27 :54-57
[3]   DRIFT Study of CuO-CeO2-TiO2 Mixed Oxides for NOx Reduction with NH3 at Low Temperatures [J].
Chen, Lei ;
Si, Zhichun ;
Wu, Xiaodong ;
Weng, Duan .
ACS APPLIED MATERIALS & INTERFACES, 2014, 6 (11) :8134-8145
[4]   DRIFT Study on Cerium-Tungsten/Titiania Catalyst for Selective Catalytic Reduction of NOx with NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (24) :9590-9596
[5]   Promotional Effect of Ce-doped V2O5-WO3/TiO2 with Low Vanadium Loadings for Selective Catalytic Reduction of NOx by NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (50) :21177-21184
[6]   Synergistic effect between the redox property and acidity on enhancing the low temperature NH3-SCR activity for NOx removal over the Co0.2CexMn0.8-xTi10 (x=0-0.40) oxides catalysts [J].
Chen, Liqiang ;
Yuan, Fulong ;
Li, Zhibin ;
Niu, Xiaoyu ;
Zhu, Yujun .
CHEMICAL ENGINEERING JOURNAL, 2018, 354 :393-406
[7]   Selective catalytic reduction of NO over carbon nanotubes supported CeO2 [J].
Chen, Xiongbo ;
Gao, Shan ;
Wang, Haiqiang ;
Liu, Yue ;
Wu, Zhongbiao .
CATALYSIS COMMUNICATIONS, 2011, 14 (01) :1-5
[8]   Characterization of ceria-coated alumina carrier [J].
Damyanova, S ;
Perez, CA ;
Schmal, M ;
Bueno, JMC .
APPLIED CATALYSIS A-GENERAL, 2002, 234 (1-2) :271-282
[9]   Promotional mechanisms of activity and SO2 tolerance of Co- or Ni-doped MnOx-CeO2 catalysts for SCR of NOx with NH3 at low temperature [J].
Gao, Fengyu ;
Tang, Xiaolong ;
Yi, Honghong ;
Li, Jingying ;
Zhao, Shunzheng ;
Wang, Jiangen ;
Chu, Chao ;
Li, Chenlu .
CHEMICAL ENGINEERING JOURNAL, 2017, 317 :20-31
[10]   The activity and characterization of CeO2-TiO2 catalysts prepared by the sol-gel method for selective catalytic reduction of NO with NH3 [J].
Gao, Xiang ;
Jiang, Ye ;
Zhong, Yi ;
Luo, Zhongyang ;
Cen, Kefa .
JOURNAL OF HAZARDOUS MATERIALS, 2010, 174 (1-3) :734-739