Comparative Studies of Effects of Vapor- and Liquid-Phase As2O3 on Catalytic Behaviors of V2O5-WO3/TiO2 Catalysts for NH3-SCR

被引:17
作者
Zhang, Handan [1 ,2 ]
Kong, Ming [1 ,2 ]
Cai, Zelong [1 ,2 ]
Liu, Qingcai [1 ,2 ]
Zeng, Jingsong [3 ]
Duan, Minghua [1 ,2 ]
Yang, Jian [1 ,2 ]
Ren, Shan [1 ,2 ]
Li, Jiangling [1 ,2 ]
机构
[1] Chongqing Univ, Coll Mat Sci & Engn, Engn Res Ctr Energy Acid Environm Chongqing, Chongqing 400044, Peoples R China
[2] Chongqing Univ, Chongqing Key Lab Vanadium Titanium Met & New Mat, Chongqing 400044, Peoples R China
[3] SPIC Yuanda Environm Protect Catalyst Co Ltd, Chongqing 401336, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
VANADIA-TITANIA CATALYSTS; COMMERCIAL SCR CATALYST; NITRIC-OXIDE; FLUE-GAS; REDUCTION; DEACTIVATION; AMMONIA; NO; MECHANISM; REGENERATION;
D O I
10.1021/acsomega.0c01734
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The role of vapor- and liquid-phase As2O3 in deactivating commercial V2O5-WO3/TiO2 catalyst during the NH3-selective catalytic reduction (SCR) process was explored and compared. As2O3 was loaded via vapor deposition (As(vap)) and the wet impregnation (As(imp)) method, respectively. Results demonstrated that the poisoning extent of vapor arsenic was much stronger than in the liquid state. Differences in As distribution on the catalyst surface was one of the main causes. Most vapor As2O3 could be oxidized to As2O5, which underwent stacking and formed a dense covering layer on the catalyst surface. In comparison, liquid As2O3 could also be oxidized but distributed uniformly and did not change the catalyst pore structure. Loading arsenic would destroy the V-OH and V=O active sites of the catalyst, and less reactive As5+-OH was generated. Catalyst oxidizability was also enhanced, resulting in NH3 oxidation enhancement, decreased N-2 selectivity, and a decline in SCR activity. Importantly, the intermediate of NH3 oxidation, NH2-amide, also could react with NO + O-2, and more N2O was generated on the poisoned catalyst during the SCR process, especially on As(imp). Finally, two mechanisms of arsenic poisoning were proposed, in which the role of vapor and liquid As2O3 over the V2O5-WO3/TiO2 catalyst was compared.
引用
收藏
页码:24195 / 24203
页数:9
相关论文
共 40 条
[1]   SELECTIVE CATALYTIC REDUCTION OF NITRIC-OXIDE WITH ETHANE AND METHANE ON SOME METAL EXCHANGED ZSM-5 ZEOLITES [J].
BURCH, R ;
SCIRE, S .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 3 (04) :295-318
[2]   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
[3]   Influence of reaction products of K-getter fuel additives on commercial vanadia-based SCR catalysts Part II. Simultaneous addition of KCl, Ca(OH)2, H3PO4 and H2SO4 in a hot flue gas at a SCR pilot-scale setup [J].
Castellino, Francesco ;
Jensen, Anker Degn ;
Johnsson, Jan Erik ;
Fehrmann, Rasmus .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 86 (3-4) :206-215
[4]   Design Strategies for P-Containing Fuels Adaptable CeO2-MoO3 Catalysts for DeNOx: Significance of Phosphorus Resistance and N2 Selectivity [J].
Chang, Huazhen ;
Jong, Min Tze ;
Wang, Chizhong ;
Qu, Ruiyang ;
Du, Yu ;
Li, Junhua ;
Hao, Jiming .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (20) :11692-11699
[5]   DEACTIVATION OF THE VANADIA CATALYST IN THE SELECTIVE CATALYTIC REDUCTION PROCESS [J].
CHEN, JP ;
BUZANOWSKI, MA ;
YANG, RT ;
CICHANOWICZ, JE .
JOURNAL OF THE AIR & WASTE MANAGEMENT ASSOCIATION, 1990, 40 (10) :1403-1409
[6]   The poisoning effect of alkali metals doping over nano V2O5-WO3/TiO2 catalysts on selective catalytic reduction of NOx by NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
CHEMICAL ENGINEERING JOURNAL, 2011, 170 (2-3) :531-537
[7]   ON THE MORPHOLOGICAL PROPERTIES OF TUNGSTA-TITANIA DE-NOXING CATALYSTS [J].
CRISTIANI, C ;
BELLOTTO, M ;
FORZATTI, P ;
BREGANI, F .
JOURNAL OF MATERIALS RESEARCH, 1993, 8 (08) :2019-2025
[8]   Investigation of the effect of Cu addition on the SO2-resistance of a Ce-Ti oxide catalyst for selective catalytic reduction of NO with NH3 [J].
Du, Xue-sen ;
Gao, Xiang ;
Cui, Li-wen ;
Fu, Yin-cheng ;
Luo, Zhong-yang ;
Cen, Ke-fa .
FUEL, 2012, 92 (01) :49-55
[9]   Molecular Transformations of Arsenic Species in the Flue Gas of Typical Power Plants: A Density Functional Theory Study [J].
Du, Xuesen ;
Tang, Jiyun ;
Gao, Xiang ;
Chen, Yanrong ;
Ran, Jingyu ;
Zhang, Li .
ENERGY & FUELS, 2016, 30 (05) :4209-4214
[10]   The Reaction of Poisonous Alkali Oxides with Vanadia SCR Catalyst and the Afterward Influence: A DFT and Experimental Study [J].
Du, Xuesen ;
Gao, Xiang ;
Qiu, Kunzan ;
Luo, Zhongyang ;
Cen, Kefa .
JOURNAL OF PHYSICAL CHEMISTRY C, 2015, 119 (04) :1905-1912