A mechanistic study of sulfur poisoning of the water-gas-shift reaction over Pd/ceria

被引：45
作者：
Luo, T [1 ]
Gorte, RJ [1 ]
机构：
[1] Univ Penn, Dept Chem Engn, Philadelphia, PA 19104 USA
来源：
CATALYSIS LETTERS | 2003年 / 85卷 / 3-4期
关键词：
ceria; SO2; cerium sulfate; water gas shift; oxygen storage capacity (OSC);
D O I：
10.1023/A:1022125209602
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：
The effect of sulfur on the water gas-shift (WGS) activity of Pd/ceria catalysts has been studied using steady-state rate measurements, pulse-reactor studies, and FTIR. After exposing Pd/ceria to SO2 at 673 K in an oxidizing environment, the WGS rates dropped to a value close to that observed on Pd/alumina. Both pulse-reactor and FTIR measurements showed that cerium sulfates can be readily reduced by CO and re-oxidized by O-2 at 723 K; however, unlike reduced ceria, the Ce2O2 S formed by reduction of the sulfates cannot be re-oxidized by H2O or CO2. The implications of these measurements for understanding the oxygen-storage capacity (OSC) of three-way catalysts are discussed.
引用
收藏
页码：139 / 146
页数：8
相关论文
共 28 条
[1]  
Bazin P, 1998, STUD SURF SCI CATAL, V116, P571
[2]   Influence of platinum on ceria sulfation [J].
Bazin, P ;
Saur, O ;
Lavalley, JC ;
Blanchard, G ;
Visciglio, V ;
Touret, O .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 13 (3-4) :265-274
[3]   Axial characterization of oxygen storage capacity in close-coupled lightoff and underfloor catalytic converters and impact of sulfur [J].
Beck, DD ;
Sommers, JW ;
DiMaggio, CL .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 11 (3-4) :273-290
[4]  
Beck DD, 1997, STUD SURF SCI CATAL, V111, P21
[5]   IMPACT OF SULFUR ON THE PERFORMANCE OF VEHICLE-AGED PALLADIUM MONOLITHS [J].
BECK, DD ;
SOMMERS, JW .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1995, 6 (02) :185-200
[6]   IMPACT OF SULFUR ON MODEL PALLADIUM-ONLY CATALYSTS UNDER SIMULATED 3-WAY OPERATION [J].
BECK, DD ;
SOMMERS, JW ;
DIMAGGIO, CL .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 3 (2-3) :205-227
[7]   Studies of the water-gas-shift reaction on ceria-supported Pt, Pd, and Rh: implications for oxygen-storage properties [J].
Bunluesin, T ;
Gorte, RJ ;
Graham, GW .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 15 (1-2) :107-114
[8]   CO oxidation for the characterization of reducibility in oxygen storage components of three-way automotive catalysts [J].
Bunluesin, T ;
Gorte, RJ ;
Graham, GW .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 14 (1-2) :105-115
[9]   Effect of ceria structure on oxygen migration for Rh/ceria catalysts [J].
Cordatos, H ;
Bunluesin, T ;
Stubenrauch, J ;
Vohs, JM ;
Gorte, RJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (02) :785-789
[10]   THERMODYNAMICS OF THE OXIDATION OF RARE-EARTH OXYSULFIDES AT HIGH-TEMPERATURES [J].
DWIVEDI, RK ;
KAY, DAR .
METALLURGICAL TRANSACTIONS B-PROCESS METALLURGY, 1984, 15 (03) :523-528
123