Iron doped effects on active sites formation over activated carbon supported Mn-Ce oxide catalysts for low-temperature SCR of NO

被引:259
作者
Yang, Jie [1 ]
Ren, Shan [1 ]
Zhang, Tianshi [1 ]
Su, Zenghui [1 ]
Long, Hongming [2 ]
Kong, Ming [1 ]
Yao, Lu [1 ]
机构
[1] Chongqing Univ, Coll Mat Sci & Engn, Chongqing 400044, Peoples R China
[2] Anhui Univ Technol, Key Lab Met Emiss Reduct & Resources Recycling, Minist Educ, Maanshan 243002, Peoples R China
基金
中国国家自然科学基金;
关键词
Low-temperature NH3-SCR; Iron doped; Activated carbon; Mn-Ce oxide catalysts; NH3-SCR REACTION; SO2; REMOVAL; SEMI-COKE; REDUCTION; NH3; MECHANISM; DRIFTS; PERFORMANCE; PROMOTION; OXYGEN;
D O I
10.1016/j.cej.2019.122398
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
To clarify the Fe doped effects over activated carbon (AC) supported Mn-Ce oxide catalysts and study the influence of Fe addition on the AC, several Mn/Ce/Fe mixed oxide catalysts prepared via an impregnation method supported on AC were investigated for low-temperature selective catalytic reduction (SCR) of NO with NH3. The Mn-Ce-Fe/AC catalyst with 5% (mass ratio) loading exhibited the highest catalytic activity and yielded above 90% NO conversion at 125 degrees C with a space velocity of 12,000 h(-1). The Fe addition could obviously reduce the destruction of AC surface area. Also, the metal ions could insert into graphite crystallite structures of AC, splitting it into smaller graphene-like sheets. After doping with Fe species, the relative ratios of Mn-4/Mnn+, Ce3+ /Cen+ and the surface adsorbed oxygen greatly enhanced in Mn-Ce-Fe/AC catalyst. Additionally, both weak acid and medium acid amount increased significantly after the Fe species introduced in Mn-Ce/AC, which could be attributed to the more exposed active sites of acid due to Fe species or its influence on Mn/Ce species. Relying on the obtained results, a L-H mechanism was proposed, owing to the Fe doping, the average valence state of Mn ions and surface adsorbed oxygen both increased on the Mn-Ce-Fe/AC catalyst, specially accompanying with the surface acid sites promotion, therefore remarkably promoting the denitration efficiency due to all the cumulative effect.
引用
收藏
页数:11
相关论文
共 44 条
[1]   Carboxylate-Assisted Transition-Metal-Catalyzed C-H Bond Functionalizations: Mechanism and Scope [J].
Ackermann, Lutz .
CHEMICAL REVIEWS, 2011, 111 (03) :1315-1345
[2]  
[Anonymous], [No title captured]
[3]   1D-MnO2, 2D-MnO2 and 3D-MnO2 for low-temperature oxidation of ethanol [J].
Bai, Bingyang ;
Li, Junhua ;
Hao, Jiming .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 164 :241-250
[4]   The characterization of activated carbons with oxygen and nitrogen surface groups [J].
Biniak, S ;
Szymanski, G ;
Siedlewski, J ;
Swiatkowski, A .
CARBON, 1997, 35 (12) :1799-1810
[5]   Influence of elevated surface texture hydrated titania on Ce-doped Mn/TiO2 catalysts for the low-temperature SCR of NOx under oxygen-rich conditions [J].
Boningari, Thirupathi ;
Ettireddy, Padmanabha R. ;
Somogyvari, Arpad ;
Liu, Yi ;
Vorontsov, Alexander ;
McDonald, Carl A. ;
Smirniotis, Panagiotis G. .
JOURNAL OF CATALYSIS, 2015, 325 :145-155
[6]   The activity and mechanism study of Fe-Mn-Ce/γ-Al2O3 catalyst for low temperature selective catalytic reduction of NO with NH3 [J].
Cao, Fan ;
Su, Sheng ;
Xiang, Jun ;
Wang, Pengying ;
Hu, Song ;
Sun, Lushi ;
Zhang, Anchao .
FUEL, 2015, 139 :232-239
[7]   Highly dispersed surface active species of Mn/Ce/TiW catalysts for high performance at low temperature NH3-SCR [J].
Chen, Hongfeng ;
Xia, Yang ;
Huang, Hui ;
Gan, Yongping ;
Tao, Xinyong ;
Liang, Chu ;
Luo, Jianmin ;
Fang, Ruyi ;
Zhang, Jun ;
Zhang, Wenkui ;
Liu, Xuesong .
CHEMICAL ENGINEERING JOURNAL, 2017, 330 :1195-1202
[8]   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
[9]   Characterization of activated carbon, graphitized carbon fibers and synthetic diamond powder using TPD and drifts [J].
Dandekar, A ;
Baker, RTK ;
Vannice, MA .
CARBON, 1998, 36 (12) :1821-1831
[10]   Ceria modified FeMnOx-Enhanced performance and sulphur resistance for low-temperature SCR of NOx [J].
France, Liam John ;
Yang, Qing ;
Li, Wan ;
Chen, Zhihang ;
Guang, Jianyu ;
Guo, Dawei ;
Wang, Lefu ;
Li, Xuehui .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 206 :203-215