Improvement in activity and alkali resistance of a novel V-Ce(SO4)2/Ti catalyst for selective catalytic reduction of NO with NH3

被引:126
作者
Hu, Wenshuo [1 ,2 ]
Zhang, Yuhong [1 ]
Liu, Shaojun [2 ,3 ]
Zheng, Chenghang [1 ]
Gao, Xiang [1 ]
Nova, Isabella [2 ]
Tronconi, Enrico [2 ]
机构
[1] Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Zhejiang, Peoples R China
[2] Politecn Milan, Lab Catalysis & Catalyt Proc, Dipartimento Energia, Via La Masa 34, I-20156 Milan, Italy
[3] Jiangsu Univ Sci & Technol, Sch Energy & Power Engn, 2 Mengxi Rd, Zhenjiang 212003, Jiangsu, Peoples R China
基金
美国国家科学基金会;
关键词
Vanadium; Ce(SO4)(2); Redox properties; Acidity; Alkali resistance; FAST SCR REACTION; V-BASED CATALYST; OXIDE CATALYST; DEACTIVATION MECHANISM; NITRIC-OXIDE; SITU-DRIFTS; AMMONIA; SPECTROSCOPY; NH3-SCR; POTASSIUM;
D O I
10.1016/j.apcatb.2017.01.036
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-Ce(SO4)(2)/Ti catalysts for selective catalytic reduction (SCR) of NO with ammonia are prepared by impregnation method. Low temperature SCR activity and alkali resistance of the optimal V-0.5Ce(SO4)(2)/Ti sample are found to be better than on the commercial V-W/Ti catalyst. Also, V-0.5Ce(SO4)(2)/Ti shows an excellent durability in the presence of SO2 and H2O, indicating to have prospects for the industrial application. Based on catalysts characterization and in-situ DRIFTS studies, a higher proportion of surface active oxygen generated by the introduction of Ce and a Much faster H-2 reduction point out the improved redox properties of V-0.5Ce(SO4)(2)/Ti, which results in a stronger NO oxidative activation and is confirmed by a more abundant formation of surface NO and NO3-species. When exposed to SCR conditions where both NH3 and NO are present, this enhanced NO activation can produce more reactive nitrite and/or NO+ intermediates which then readily react with adsorbed NH3 and decorripose to N-2 and H2O, accounting for the improved SCR activity of V-0.5Ce(SO4)(2)/Ti at low temperatures. The addition of Ce(SO4)(2) also provides abundant reactive acid sites and adsorbed NH3 species thus increase. Even after Na poisoning, adequate surface acidity and redox properties still remain. Furthermore, relatively higher contents of V-OH are preserved owing to the interaction between Na and O=S=O, acting as a protection for the active sites. These promotional effects contribute to the better alkali resistance of V-0.5Ce(SO4)(2)/Ti. Therefore, all the results suggest that V-0.5Ce(SO4)(2)/Ti is a promising candidate as a catalyst for NH3-SCR in coal-fired power plants, especially under high Na-content conditions. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:449 / 460
页数:12
相关论文
共 40 条
[1]   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
[2]   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
[3]   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
[4]   Promotional Effect of Ce-doped V2O5-WO3/TiO2 with Low Vanadium Loadings for Selective Catalytic Reduction of NOx by NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (50) :21177-21184
[5]  
Choo ST, 2000, APPL CATAL A-GEN, V200, P177, DOI 10.1016/S0926-860X(00)00636-0
[6]   Reactivity of NO/NO2-NH3 SCR system for diesel exhaust aftertreatment:: Identification of the reaction network as a function of temperature and NO2 feed content [J].
Ciardelli, Cristian ;
Nova, Isabella ;
Tronconi, Enrico ;
Chatterjee, Daniel ;
Bandl-Konrad, Brigitte ;
Weibel, Michel ;
Krutzsch, Bernd .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2007, 70 (1-4) :80-90
[7]   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
[8]   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
[9]   The Influence of Alkali Metals on the Ce-Ti Mixed Oxide Catalyst for the Selective Catalytic Reduction of NOx [J].
Du, Xuesen ;
Gao, Xiang ;
Qu, Ruiyang ;
Ji, Peidong ;
Luo, Zhongyang ;
Cen, Ke-fa .
CHEMCATCHEM, 2012, 4 (12) :2075-2081
[10]   Enhanced NH3 Selective Catalytic Reduction for NOx Abatement [J].
Forzatti, Pio ;
Nova, Isabella ;
Tronconi, Enrico .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (44) :8366-8368