Theoretical and experimental study on the deactivation of V2O5 based catalyst by lead for selective catalytic reduction of nitric oxides

被引:120
作者
Gao, Xiang [1 ]
Du, Xue-sen [1 ]
Fu, Yin-cheng [1 ]
Mao, Jian-hong [1 ]
Luo, Zhong-yang [1 ]
Ni, Ming-jiang [1 ]
Cen, Ke-fa [1 ]
机构
[1] Zhejiang Univ, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China
基金
中国国家自然科学基金;
关键词
Selective catalytic reduction; Deactivation; Lead; Density functional theory; V2O5; V2O5/WO3-TIO2 SCR CATALYSTS; DENSITY-FUNCTIONAL THEORY; GETTER FUEL ADDITIVES; VANADIUM-OXIDE; CHEMICAL DEACTIVATION; REACTION-PRODUCTS; LUBRICATION OILS; CLUSTER MODEL; UREA SOLUTION; ALKALI;
D O I
10.1016/j.cattod.2011.05.025
中图分类号
O69 [应用化学];
学科分类号
070301 [无机化学];
摘要
A combination of theoretical and experimental methods, including DFT calculation, BET, Raman spectroscopy, NH3-TPD, H-2-TPR and XPS, has been used to elucidate the mechanism of lead deactivating effect on the V2O5 based SCR catalyst. The theoretical calculations have shown that the doping of lead atom will cause the great change of the surface electronic property. Each lead atom will influence two active sites, resulting in the decrease of the acid formability and reducibility of the catalyst surface. The NH3-TPD and H-2-TPR experiments have shown the decrease of acid site amount and reducibility, which is in accordance with the calculation result. The BET result has also shown the physical influence caused by the doping of lead compound. The NO conversion experiment has confirmed the deactivation effect of lead on the V2O5 based catalyst. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:625 / 630
页数:6
相关论文
共 28 条
[1]
Density functional theory studies of mechanistic aspects of the SCR reaction on vanadium oxide catalysts [J].
Anstrom, M ;
Topsoe, NY ;
Dumesic, JA .
JOURNAL OF CATALYSIS, 2003, 213 (02) :115-125
[2]
DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[3]
DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].
BECKE, AD .
PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100
[4]
The role of tungsten in formation of active sites for no SCR on the V-W-O catalyst surface -: quantum chemical modeling (DFT) [J].
Broclawik, E ;
Góra, A ;
Najbar, M .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2001, 166 (01) :31-38
[5]
Influence of reaction products of K-getter fuel additives on commercial vanadia-based SCR catalysts Part I. Potassium phosphate [J].
Castellino, Francesco ;
Jensen, Anker Degn ;
Johnsson, Jan Erik ;
Fehrmann, Rasmus .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 86 (3-4) :196-205
[6]
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
[7]
Analysis of silica-supported vanadia by X-ray absorption spectroscopy: Combined theoretical and experimental studies [J].
Cavalleri, M. ;
Hermann, K. ;
Knop-Gericke, A. ;
Haevecker, M. ;
Herbert, R. ;
Hess, C. ;
Oestereich, A. ;
Doebler, J. ;
Schloegl, R. .
JOURNAL OF CATALYSIS, 2009, 262 (02) :215-223
[8]
Geometric and electronic structure of vanadium pentoxide: A density functional bulk and surface study [J].
Chakrabarti, A ;
Hermann, K ;
Druzinic, R ;
Witko, M ;
Wagner, F ;
Petersen, M .
PHYSICAL REVIEW B, 1999, 59 (16) :10583-10590
[9]
MECHANISM OF POISONING OF THE V2O5 TIO2 CATALYST FOR THE REDUCTION OF NO BY NH3 [J].
CHEN, JP ;
YANG, RT .
JOURNAL OF CATALYSIS, 1990, 125 (02) :411-420
[10]
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