Effect of temperature, steam-to-carbon ratio, and alkali metal additives on improving the sulfur tolerance of a Rh/La-Al2O3 catalyst reforming gasoline for fuel cell applications

被引:49
作者
Ferrandon, Magali [1 ]
Mawdsley, Jennifer [1 ]
Krause, Theodore [1 ]
机构
[1] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60430 USA
关键词
Rh; reforming; gasoline; sulfur; poisoning; deactivation; coke; SEM;
D O I
10.1016/j.apcata.2008.03.001
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 [物理化学]; 081704 [应用化学];
摘要
2 wt% Rh/La-Al2O3 Was tested for autothermal reforming (ATR) of S-free and 34 ppm-S-gasoline and characterized by scanning electron microscopy, elemental analyses, surface area, CO chemisorption, DRIFTS and X-ray absorption spectroscopy. The poisoning effect of S was more pronounced during ATR at 700 degrees C than at 800 degrees C. Complete recovery of the initial activity could be achieved when switching from S-containing gasoline to S-free gasoline at 800 degrees C, while only 50% of the activity could be recovered at 700 degrees C. Sulfur increased Rh sintering due to an increase in the catalyst temperature caused by a greater inhibition of steam reforming than partial oxidation. An increase in the H2O:C from 2.0 to 3.0, or the addition of K to Rh significantly enhanced the sulfur tolerance of the catalysts. The beneficial effect of temperature, steam, and alkali metal was attributed to the inhibition of coke, which was the major cause of catalyst deactivation. Published by Elsevier B.V.
引用
收藏
页码:69 / 77
页数:9
相关论文
共 24 条
[1]
Development of ceria-supported sulfur tolerant nanocatalysts: Rh-based formulations [J].
Azad, Abdul-Majeed ;
Duran, Martin J. .
APPLIED CATALYSIS A-GENERAL, 2007, 330 (1-2) :77-88
[2]
Mechanisms of catalyst deactivation [J].
Bartholomew, CH .
APPLIED CATALYSIS A-GENERAL, 2001, 212 (1-2) :17-60
[3]
SULFUR POISONING OF METALS [J].
BARTHOLOMEW, CH ;
AGRAWAL, PK ;
KATZER, JR .
ADVANCES IN CATALYSIS, 1982, 31 :135-242
[4]
Catalytic autothermal reforming of diesel fuel for hydrogen generation in fuel cells II. Catalyst poisoning and characterization studies [J].
Cheekatamarla, PK ;
Lane, AM .
JOURNAL OF POWER SOURCES, 2006, 154 (01) :223-231
[5]
Catalytic autothermal reforming of diesel fuel for hydrogen generation in fuel cells - I. Activity tests and sulfur poisoning [J].
Cheekatamarla, PK ;
Lane, AM .
JOURNAL OF POWER SOURCES, 2005, 152 (01) :256-263
[6]
RESISTIVITY TO SULFUR POISONING OF NICKEL ALUMINA CATALYSTS [J].
CHEN, IW ;
SHIUE, DW .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1988, 27 (08) :1391-1396
[7]
EFFECT OF SULFUR ON THE COKING OF RHODIUM IN THE STEAM REFORMING OF 1-METHYLNAPHTHALENE [J].
DELAHAY, G ;
DUPREZ, D .
APPLIED CATALYSIS, 1989, 53 (01) :95-105
[8]
Influence of alkali additives on activity and toxicity of H2S and thiophene over a Ni/SiO2 catalyst [J].
Diaz, A ;
Odriozola, JA ;
Montes, M .
APPLIED CATALYSIS A-GENERAL, 1998, 166 (01) :163-172
[9]
In situ EXAFS study of Rh/Al2O3 catalysts for catalytic partial oxidation of methane [J].
Grunwaldt, JD ;
Basini, L ;
Clausen, BS .
JOURNAL OF CATALYSIS, 2001, 200 (02) :321-329
[10]
DIFFUSE REFLECTANCE FT-IR STUDIES OF THE ADSORPTION OF CO ON RH/AL2O3 CATALYSTS [J].
HAMADEH, IM ;
GRIFFITHS, PR .
APPLIED SPECTROSCOPY, 1987, 41 (04) :682-688