Simultaneous removal of elemental mercury and NO in simulated flue gas over V2O5/ZrO2-CeO2 catalyst

被引:170
作者
Zhao, Lingkui [1 ,2 ]
Li, Caiting [1 ,2 ]
Li, Shanhong [1 ,2 ]
Wang, Yan [1 ,2 ]
Zhang, Junyi [1 ,2 ]
Wang, Teng [1 ,2 ]
Zeng, Guangming [1 ,2 ]
机构
[1] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China
[2] Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China
基金
中国国家自然科学基金;
关键词
V2O5; Elemental mercury; NH3-SCR; CeO2-ZrO2; Nitrogen oxide; MIXED-OXIDE CATALYST; HYDROTHERMAL STABILITY; V2O5-WO3/TIO2; CATALYST; INTEGRATIVE PROCESS; MNOX-CEO2; CE-ZR; REDUCTION; OXIDATION; SO2; NH3;
D O I
10.1016/j.apcatb.2016.05.079
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 V/ZrCex catalyst synthesized by a co-precipitation method was employed to investigate the simultaneous removal of NO and elemental mercury (Hg-0) in simulated flue gas. The catalysts were characterized using BET, SEM, XRD, H-2-TPR, XPS, and FT-IR. V/ZrCe0.6 with CeO2/ZrO2 molar ratio of 0.6 showed excellent SCR activity (87.3%) and high Hg oxidation efficiency (77.6%) in SCR atmosphere (NH3/NO = 1). The results indicated that the Hg had little impact on NO conversion, while the coexistence of NO and O-2 would be beneficial for the Hg oxidation. Hg oxidation was inhibited in SCR atmosphere owing to the presence of NH3. The characterization results demonstrated that the superior performance of V/ZrCe0.6 catalyst might be attributed to lower crystallinity, better texture properties, strong redox ability and high reactive nitrate together with NH3 species. The redox equilibrium (Ce3+ + V5+ <-> Ce4+ + V4+) contributed to the NO conversion and Hg oxidation. The bidentate sulfates formed by adsorbed SO2 could provide new acid sites for NH3 adsorption and increase the amount of NH4+, which reduced the poisoning effect of SO2 and H2O. Based on the experimental results, a mechanism for the simultaneous removal of NO and Hg was proposed for the V/ZrCe0.6 catalysts: 2NH(3)/NH4+(ad) + NO2(ad) + NO(g) -> 2N(2) + 3H(2)O+/2H(+), Hg(ad)+O beta -> HgO(ad). (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:420 / 430
页数:11
相关论文
共 84 条
[1]   FT-IR spectroscopic and catalytic study of de-aluminated H-mordenites as environmental friendly catalysts in the hydroxymethylation of 2-methoxyphenol with formaldehyde in aqueous medium [J].
Armandi, M. ;
Bonelli, B. ;
Garrone, E. ;
Ardizzi, M. ;
Cavani, F. ;
Dal Pozzo, L. ;
Maselli, L. ;
Mezzogori, R. ;
Calestani, G. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2007, 70 (1-4) :585-596
[2]   Selective catalytic reduction of nitric oxide with ammonia over zirconium-doped copper/ZSM-5 catalysts [J].
Bin, Feng ;
Song, Chonglin ;
Lv, Gang ;
Song, Jinou ;
Wu, Shaohua ;
Li, Xiaodong .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 150 :532-543
[3]   Performance of V2O5/NPTiO2-Al2O3-nanoparticle- and V2O5/NTiO2-Al2O3-nanotube model catalysts in the SCR-NO with NH3 [J].
Camposeco, R. ;
Castillo, S. ;
Mejia-Centeno, Isidro .
CATALYSIS COMMUNICATIONS, 2015, 60 :114-119
[4]   Composition dependent performance of alumina-based oxide supported WO3 catalysts for the NH3-SCR reaction and the NSR plus SCR coupled process [J].
Can, Fabien ;
Courtois, Xavier ;
Berland, Sebastien ;
Seneque, Mickael ;
Royer, Sebastien ;
Duprez, Daniel .
CATALYSIS TODAY, 2015, 257 :41-50
[5]   Characterization of Nb-Containing MnOx-CeO2 Catalyst for Low-Temperature Selective Catalytic Reduction of NO with NH3 [J].
Casapu, Maria ;
Kroecher, Oliver ;
Mehring, Max ;
Nachtegaal, Maarten ;
Borca, Camelia ;
Harfouche, Messaoud ;
Grolimund, Daniel .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (21) :9791-9801
[6]   Design Strategies for CeO2-MoO3 Catalysts for DeNOx and Hg0 Oxidation in the Presence of HCl: The Significance of the Surface Acid-Base Properties [J].
Chang, Huazhen ;
Wu, Qingru ;
Zhang, Tao ;
Li, Mingguan ;
Sun, Xiaoxu ;
Li, Junhua ;
Duan, Lei ;
Hao, Jiming .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2015, 49 (20) :12388-12394
[7]   Improvement of Activity and SO2 Tolerance of Sn-Modified MnOx-CeO2 Catalysts for NH3-SCR at Low Temperatures [J].
Chang, Huazhen ;
Chen, Xiaoyin ;
Li, Junhua ;
Ma, Lei ;
Wang, Chizhong ;
Liu, Caixia ;
Schwank, Johannes W. ;
Hao, Jiming .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (10) :5294-5301
[8]   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
[9]   Mechanism of the Selective Catalytic Oxidation of Slip Ammonia over Ru-Modified Ce-Zr Complexes Determined by in Situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy [J].
Chen, Wanmiao ;
Ma, Yongpeng ;
Qu, Zan ;
Liu, Qinghang ;
Huang, Wenjun ;
Hu, Xiaofang ;
Yan, Naiqiang .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2014, 48 (20) :12199-12205
[10]   Promotional effect of Nb additive on the activity and hydrothermal stability for the selective catalytic reduction of NOx with NH3 over CeZrOx catalyst [J].
Ding, Shipeng ;
Liu, Fudong ;
Shi, Xiaoyan ;
He, Hong .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2016, 180 :766-774