"Fast SCR" reaction over Sm-modified MnOx-TiO2 for promoting reduction of NOx with NH3

被引:154
作者
Gao, Chen [1 ]
Shi, Jian-Wen [1 ]
Fan, Zhaoyang [1 ]
Wang, Baorui [1 ]
Wang, Yao [1 ]
He, Chi [2 ]
Wang, Xinbo [1 ]
Li, Jun [1 ]
Niu, Chunming [1 ]
机构
[1] Xi An Jiao Tong Univ, Ctr Nanomat Renewable Energy, State Key Lab Elect Insulat & Power Equipment, Sch Elect Engn, Xian 710049, Shaanxi, Peoples R China
[2] Xi An Jiao Tong Univ, Dept Environm Sci & Engn, Sch Energy & Power Engn, Xian 710049, Shaanxi, Peoples R China
关键词
Selective catalytic reduction; MnOx; Fast SCR; Reaction mechanism; de-NOx; SELECTIVE CATALYTIC-REDUCTION; LOW-TEMPERATURE; MANGANESE OXIDES; REACTION-MECHANISM; CARBON NANOTUBES; MNOX CATALYSTS; SO2; TOLERANCE; MIXED OXIDES; NH3-SCR; OXIDATION;
D O I
10.1016/j.apcata.2018.07.017
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 series of Sm-modified MnOx-TiO2 (SMT) catalysts are prepared and characterized. The results show that the introduction of Sm can effectively restrain the crystallization process of MnOx and TiO2, enhance the specific surface area, increase the surface concentration of chemisorbed oxygen species and the amount of strong surface acid sites, and reduce the surface concentration of Mn4+. The catalytic performances of the SMT catalysts are evaluated by the selective catalytic reduction (SCR) of NOx with NH3. It is found that SMT-0.3 catalyst (a 0.3 mol rate of Sm/Mn) exhibits a 100% N-x conversion in a wide operating temperature window from 180 to 390 degrees C, and a 100% N-2 selectivity from 120 to 390 degrees C under a GHSV of 36,000 h(-1), which is obviously better than MnOx TiO2 without Sm addition. In-situ DRIFT spectra reveal that, at low temperature (below 200 degrees C), absorbed NH3 species can react with gas-phase NO over MnOx-TiO2 catalyst following Eley-Rideal (E-R) mechanism, while the NH3-SCR of NO over SMT-0.3 follows both E-R and Langmuir-Hinshelwood (L-H) mechanisms. However, at high temperature (above 200 degrees C), the SCR reaction over MnOx-TiO2 is via "standard SCR" process, but the SCR reaction over SMT-0.3 is through "fast SCR" reaction.
引用
收藏
页码:102 / 112
页数:11
相关论文
共 72 条
[1]   Impact of nitrogen oxides on the environment and human health: Mn-based materials for the NOx abatement [J].
Boningari, Thirupathi ;
Smirniotis, Panagiotis G. .
CURRENT OPINION IN CHEMICAL ENGINEERING, 2016, 13 :133-141
[2]   Influence of SiO2 on MiTiO2 (M = Cu, Mn, and Ce) Formulations for Low-Temperature Selective Catalytic Reduction of NOx with NH3: Surface Properties and Key Components in Relation to the Activity of NOx Reduction [J].
Boningari, Thirupathi ;
Pappas, Dimitrios K. ;
Ettireddy, Padmanabha R. ;
Kotrba, Adam ;
Smirniotis, Panagiotis G. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2015, 54 (08) :2261-2273
[3]   Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:: A review [J].
Busca, G ;
Lietti, L ;
Ramis, G ;
Berti, F .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 18 (1-2) :1-36
[4]   Ge, Mn-doped CeO2-WO3 catalysts for NH3-SCR of NOx: Effects of SO2 and H2 regeneration [J].
Chang, Huazhen ;
Li, Junhua ;
Yuan, Jian ;
Chen, Liang ;
Dai, Yun ;
Arandiyan, Hamidreza ;
Xu, Jiayu ;
Hao, Jiming .
CATALYSIS TODAY, 2013, 201 :139-144
[5]   CeO2-WO3 Mixed Oxides for the Selective Catalytic Reduction of NOx by NH3 Over a Wide Temperature Range [J].
Chen, Liang ;
Li, Junhua ;
Ablikim, Wijdan ;
Wang, Jun ;
Chang, Huazhen ;
Ma, Lei ;
Xu, Jiayu ;
Ge, Maofa ;
Arandiyan, Hamidreza .
CATALYSIS LETTERS, 2011, 141 (12) :1859-1864
[6]   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
[7]   Promoting catalytic performances of Ni-Mn spinel for NH3-SCR by treatment with SO2 and H2O [J].
Chen, Liqiang ;
Niu, Xiaoyu ;
Li, Zhibin ;
Dong, Yongli ;
Zhang, Zhiping ;
Yuan, Fulong ;
Zhu, Yujun .
CATALYSIS COMMUNICATIONS, 2016, 85 :48-51
[8]   Promoting effect of Nd on the reduction of NO with NH3 over CeO2 supported by activated semi-coke: an in situ DRIFTS study [J].
Chen, Yan ;
Wang, Jinping ;
Yan, Zheng ;
Liu, Lili ;
Zhang, Zuotai ;
Wang, Xidong .
CATALYSIS SCIENCE & TECHNOLOGY, 2015, 5 (04) :2251-2259
[9]   Rationally Designed Porous MnOx-FeOx Nanoneedles for Low-Temperature Selective Catalytic Reduction of NOx by NH3 [J].
Fan, Zhaoyang ;
Shi, Jian-Wen ;
Gao, Chen ;
Gao, Ge ;
Wang, Baorui ;
Niu, Chunming .
ACS APPLIED MATERIALS & INTERFACES, 2017, 9 (19) :16117-16127
[10]   Sulfur and Water Resistance of Mn-Based Catalysts for Low-Temperature Selective Catalytic Reduction of NOx: A Review [J].
Gao, Chen ;
Shi, Jian-Wen ;
Fan, Zhaoyang ;
Gao, Ge ;
Niu, Chunming .
CATALYSTS, 2018, 8 (01)