DRIFTS study of the catalytic N2O reduction by SO2 on FeZSM-5

被引:10
作者
Abello, Sonia [1 ]
Hevia, Miguel A. G. [1 ]
Santiago, Marta [1 ]
Perez-Ramirez, Javier [1 ,2 ]
机构
[1] Inst Chem Res Catalonia ICIQ, Tarragona 43007, Spain
[2] Catalan Inst Res & Adv Studies ICREA, Barcelona 08010, Spain
关键词
N2O abatement; SO2; Iron zeolites; FeZSM-5; Sulfate; Infrared spectroscopy; ACTIVATED FEMFI ZEOLITES; NITROUS-OXIDE; SULFUR-DIOXIDE; DECOMPOSITION; REMOVAL; BEHAVIOR; H2O; NOX; CO; MECHANISM;
D O I
10.1016/j.catcom.2010.05.009
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
SO2 has been recognized as an effective reducing agent for N2O over iron-containing zeolite catalysts, lowering the operation temperature up to 100 K with respect to the direct N2O decomposition. This unique behavior contrasts with the common poisoning effect of SO2 over other active de-N2O metals (e.g. Co, Cu, Rh, and Ru). The formation of surface sulfates has been generally posed as the main cause for catalyst deactivation by SO2. Through the use of in situ infrared spectroscopy (DRIFTS), we show that steam-activated FeZSM-5 indeed builds up stable sulfate species during the N2O + SO2 reaction. Significant amounts of sulfur were detected in the used catalyst by elemental analysis and X-ray photoelectron spectroscopy. However, the enhanced N2O conversion is remarkably stable, indicating that the reducing action by SO2 and the sulfation of the surface are decoupled. The resulting sulfate species are thus spectators in the catalytic process and do not block or alter the structure of the active sites for N2O reduction and decomposition. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:1058 / 1062
页数:5
相关论文
共 31 条
[21]   Steam-activated FeMFI zeolites.: Evolution of iron species and activity in direct N2O decomposition [J].
Pérez-Ramírez, J ;
Kapteijn, F ;
Groen, JC ;
Doménech, A ;
Mul, G ;
Moulijn, JA .
JOURNAL OF CATALYSIS, 2003, 214 (01) :33-45
[22]   Physicochemical characterization of isomorphously substituted FeZSM-5 during activation [J].
Pérez-Ramírez, J ;
Mul, G ;
Kapteijn, F ;
Moulijn, JA ;
Overweg, AR ;
Doménech, A ;
Ribera, A ;
Arends, IWCE .
JOURNAL OF CATALYSIS, 2002, 207 (01) :113-126
[23]   High activity and stability of the Rh-free Co-based ex-hydrotalcite containing Pd in the catalytic decomposition of N2O [J].
Pérez-Ramírez, J ;
Kapteijn, F ;
Moulijn, JA .
CATALYSIS LETTERS, 1999, 60 (03) :133-138
[24]   Highly active SO2-resistant ex-framework FeMFI catalysts for direct N2O decomposition [J].
Pérez-Ramírez, J ;
Kapteijn, F ;
Mul, G ;
Moulijn, JA .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2002, 35 (03) :227-234
[25]   SO2-promoted catalytic N2O removal over iron zeolites [J].
Perez-Ramirez, Javier ;
Hevia, Miguel A. G. ;
Abello, Sonia .
CHEMICAL COMMUNICATIONS, 2008, (42) :5351-5353
[26]   Evaluation of catalysts for N2O abatement in fluidized-bed combustion [J].
Santiago, Marta ;
Hevia, Miguel A. G. ;
Perez-Ramirez, Javier .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 90 (1-2) :83-88
[27]   Decomposition of the sulfates of copper, iron (II), iron (III), nickel, and zinc: XPS, SEM, DRIFTS, XRD, and TGA study [J].
Siriwardane, RV ;
Poston, JA ;
Fisher, EP ;
Shen, MS ;
Miltz, AL .
APPLIED SURFACE SCIENCE, 1999, 152 (3-4) :219-236
[28]   Study of ceria sulfation [J].
Waqif, M ;
Bazin, P ;
Saur, O ;
Lavalley, JC ;
Blanchard, G ;
Touret, O .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 11 (02) :193-205
[29]   NATURE AND MECHANISM OF FORMATION OF SULFATE SPECIES ON COPPER ALUMINA SORBENT CATALYSTS FOR SO2 REMOVAL [J].
WAQIF, M ;
SAUR, O ;
LAVALLEY, JC ;
PERATHONER, S ;
CENTI, G .
JOURNAL OF PHYSICAL CHEMISTRY, 1991, 95 (10) :4051-4058
[30]   Simultaneous removal of SO2 and NOx from flue gas using a CuO/Al2O3 catalyst sorbent II.: Promotion of SCR activity by SO2 at high temperatures [J].
Xie, GY ;
Liu, ZY ;
Zhu, ZP ;
Liu, QY ;
Ge, J ;
Huang, ZG .
JOURNAL OF CATALYSIS, 2004, 224 (01) :42-49