Catalytic active site for NO decomposition elucidated by surface science and real catalyst

被引:19
作者
Haneda, M [1 ]
Nakamura, I [1 ]
Fujitani, T [1 ]
Hamada, H [1 ]
机构
[1] AIST, Res Inst Innovat Sustainable Chem, Tsukuba, Ibaraki 3058565, Japan
关键词
NO decomposition; surface science; single-crystal; powder catalysts;
D O I
10.1007/s10563-005-9156-1
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
Comprehensive studies combining surface science and real catalyst were performed to get further insight into catalytic active site and reaction mechanism for NO decomposition over supported palladium and cobalt oxide-based catalysts. On palladium single-crystal model catalysts, adsorption, dissociation and desorption behavior of NO was found to be closely related to the surface structures, the stepped surface palladium being active for dissociation of NO. In accordance with this result, the activity of powder Pd/Al2O3 catalysts for NO decomposition was directly related to the number of step sites exposed on the surface, suggesting that the step sites act as the catalytic active site for NO decomposition on Pd/Al2O3. NO decomposition over cobalt oxide was found to be significantly promoted by addition of alkali metals. Surface science study and catalyst characterization led to the same conclusion that the interface between the alkali metal and Co3O4 serves as the catalytic active site. From the results of in situ Fourier transform infrared (FT-IR) spectroscopy and isotopic transient kinetic analysis, a reaction mechanism was proposed in which the reaction is initiated by NO adsorption onto alkali metals to form NO2- species and then NO2- species react with the adsorbed NO species to form N-2 over the interface between the alkali metal and Co3O4.
引用
收藏
页码:207 / 215
页数:9
相关论文
共 29 条
[1]   ACTIVATION OF NITROGEN BY ALKALI-METAL PROMOTED TRANSITION-METAL .1. AMMONIA SYNTHESIS OVER RUTHENIUM PROMOTED BY ALKALI-METAL [J].
AIKA, K ;
OZAKI, A ;
HORI, H .
JOURNAL OF CATALYSIS, 1972, 27 (03) :424-&
[2]   X-RAY PHOTOEMISSION SPECTROSCOPY OF POTASSIUM PROMOTED FE AND PT SURFACES AFTER H-2 REDUCTION AND CO/H-2 REACTION [J].
BONZEL, HP ;
BRODEN, G ;
KREBS, HJ .
APPLICATIONS OF SURFACE SCIENCE, 1983, 16 (3-4) :373-394
[3]   Heterogeneous molecular catalysis: Oxymoron or reality? [J].
Boudart, M .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1997, 120 (1-3) :271-280
[4]   NO chemisorption and reactions on metal surfaces: A new perspective [J].
Brown, WA ;
King, DA .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (12) :2578-2595
[5]   EFFECT OF PRECURSOR ON THE CATALYTIC BEHAVIOR OF RU-CU/MGO [J].
CRISAFULLI, C ;
MAGGIORE, R ;
SCIRE, S ;
SOLARINO, L ;
GALVAGNO, S .
JOURNAL OF MOLECULAR CATALYSIS, 1990, 63 (01) :55-63
[6]   THEORY OF ATOM-METAL INTERACTIONS .I. ALKALI ATOM ADSORPTION [J].
GADZUK, JW .
SURFACE SCIENCE, 1967, 6 (02) :133-&
[7]   Mechanism of NOx decomposition [J].
Garin, F .
APPLIED CATALYSIS A-GENERAL, 2001, 222 (1-2) :183-219
[8]   Identification of neutral and charged NxOy surface species by IR spectroscopy [J].
Hadjiivanov, KI .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2000, 42 (1-2) :71-144
[9]   Reaction mechanism of NO decomposition over alkali metal-doped cobalt oxide catalysts [J].
Haneda, M ;
Kintaichi, Y ;
Hamada, H .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 55 (03) :169-175
[10]   Alkali metal-doped cobalt oxide catalysts for NO decomposition [J].
Haneda, M ;
Kintaichi, Y ;
Bion, N ;
Hamada, H .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 46 (03) :473-482