Exploration of reaction mechanism between acid gases and elemental mercury on the CeO2-WO3/TiO2 catalyst via in situ DRIFTS

被引:48
作者
Li, Guoliang [1 ,2 ]
Wang, Shuxiao [1 ,2 ]
Wu, Qingru [1 ,2 ]
Li, Junhua [1 ,2 ]
You, Xiaoqing [3 ,4 ]
Shao, Sen [3 ,4 ]
Liu, Kaiyun [1 ,2 ]
机构
[1] Tsinghua Univ, State Key Joint Lab Environm Simulat & Pollut Con, Sch Environm, Beijing 100084, Peoples R China
[2] State Environm Protect Key Lab Sources & Control, Beijing 100084, Peoples R China
[3] Tsinghua Univ, Minist Educ, Key Lab Thermal Sci & Power Engn, Beijing 100084, Peoples R China
[4] Tsinghua Univ, Ctr Combust Energy, Beijing 100084, Peoples R China
基金
美国国家科学基金会;
关键词
Mercury oxidation; CeO2; catalyst; HCl; NO; SO2; FLUE-GAS; SIMULTANEOUS REMOVAL; SO2; RESISTANCE; SCR CATALYST; OXIDATION; REDUCTION; NO; COMPONENTS; EMISSIONS; HG-0;
D O I
10.1016/j.fuel.2018.10.142
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Although the oxidation of elemental mercury (Hg-0) on catalyst can be significantly affected by acid gases, its mechanism is still unclear. This study used in situ DRIFT to research the influence of acid gases (NO, HCl and SO2) on the performance of mercury oxidation on catalyst CeO2(5)-WO3(9)/TiO2. The catalyst could capture a large amount of Hg-0 on the surface yet not oxidize all Hg-0 into gaseous oxidation mercury (Hg2+) due to the limit of oxidation sites (CeO2). The addition of NO and HCl improved the mercury oxidation efficiency because this process transformed the adsorbed mercury on the catalyst into gaseous Hg2+ and formed new active sites. The in situ DRIFTS result indicated that NO2 and nitrate served as active sites for mercury oxidation. The formation of active chlorine (Cl*) via HCl adsorption on the catalyst promoted the transformation of mercury into gaseous HgCl2. The NO and HCl addition could keep the mercury oxidation efficiency over 91.5% with the presence of 500-3000 ppm SO2 and increase the SO2 resistance of the catalyst. The reaction of NO and Hg-0 conforms to the Eley-Ridcal mechanism, while the reaction of HCl and Hg-0 follows the Languir-Hinshelwood mechanism.
引用
收藏
页码:162 / 172
页数:11
相关论文
共 44 条
[1]   XPS and XAS study of the sorption of Hg(II) onto pyrite [J].
Behra, P ;
Bonnissel-Gissinger, P ;
Alnot, M ;
Revel, R ;
Ehrhardt, JJ .
LANGMUIR, 2001, 17 (13) :3970-3979
[2]   Abatement of mercury emissions in the coal combustion process equipped with a Fabric Filter Baghouse [J].
Cao, Yan ;
Cheng, Chin-Min ;
Chen, Chien-Wei ;
Liu, Mingchong ;
Wang, Chiawei ;
Pan, Wei-Ping .
FUEL, 2008, 87 (15-16) :3322-3330
[3]   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
[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]   Novel Effective Catalyst for Elemental Mercury Removal from Coal-Fired Flue Gas and the Mechanism Investigation [J].
Chen, Wanmiao ;
Pei, Yang ;
Huang, Wenjun ;
Qu, Zan ;
Hu, Xiaofang ;
Yan, Naiqiang .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2016, 50 (05) :2564-2572
[6]   The effect of oxygen concentration on the reduction of NO with propylene over CuO/γ-Al2O3 [J].
Chi, Y ;
Chuang, SSC .
CATALYSIS TODAY, 2000, 62 (04) :303-318
[7]   A Critical Review on the Heterogeneous Catalytic Oxidation of Elemental Mercury in Flue Gases [J].
Gao, Yanshan ;
Zhang, Zhang ;
Wu, Jingwen ;
Duan, Linhai ;
Umar, Ahmad ;
Sun, Luyi ;
Guo, Zhanhu ;
Wang, Qiang .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (19) :10813-10823
[8]   Elemental mercury removal by CeO2/TiO2-PILCs under simulated coal-fired flue gas [J].
He, Chuan ;
Shen, Boxiong ;
Chi, Guilong ;
Li, Fukuan .
CHEMICAL ENGINEERING JOURNAL, 2016, 300 :1-8
[9]   Effects of flue gas components on removal of elemental mercury over Ce-Mnox/Ti-PILCs [J].
He, Chuan ;
Shen, Boxiong ;
Li, Fukuan .
JOURNAL OF HAZARDOUS MATERIALS, 2016, 304 :10-17
[10]   Adsorption and Oxidation of Elemental Mercury over Ce-MnOx/Ti-PILCs [J].
He, Chuan ;
Shen, Boxiong ;
Chen, Jianhong ;
Cai, Ji .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2014, 48 (14) :7891-7898