Effect of sulfur in catalytic partial oxidation of methane over Rh-Ce coated foam monoliths

被引：55

作者：

Bitsch-Larsen, A. ^{[1
]}

Degenstein, N. J. ^{[1
]}

Schmidt, L. D. ^{[1
]}

机构：

[1] Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55455 USA

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2008年 / 78卷 / 3-4期

关键词：

catalytic partial oxidation; methane; rhodium; ceria; sulfur poisoning; steam reforming;

D O I：

10.1016/j.apcatb.2007.09.006

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 potentially important technology to convert natural gas to syngas is catalytic partial oxidation (CPO) over precious metal catalysts. However, natural gas contains small amounts of sulfur compounds which can poison the catalyst. It is therefore of interest to investigate the effect of sulfur on the performance of CPO. In this work CPO experiments have been performed over Rh-Ce coated foam monoliths with CH3SH added to methane. The result of ppm levels of sulfur is a large (similar to 200 degrees C) temperature increase, along with lower methane conversion and lower hydrogen selectivity. A doubling of the sulfur level from 14 to 28 ppm does not result in significant changes, showing that the effect saturates at a few ppm. The poisoning effect has been investigated by analyzing both effluent and spatially resolved data and is shown to be due to severe hindrance of steam reforming by adsorbed sulfur. (c) 2007 Elsevier B.V. All rights reserved.

引用

页码：364 / 370

页数：7

共 21 条

[1] CO2 reforming of CH4 [J].

Bradford, MCJ ;

Vannice, MA .

CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1999, 41 (01) :1-42

[2] Oxy-methane reforming over high temperature stable NiCoMgCeOx and NiCoMgOx supported on zirconia-haffnia catalysts:: Accelerated sulfur deactivation and regeneration [J].

Choudhary, V. R. ;

Mondal, K. C. ;

Chouldhary, T. V. .

CATALYSIS COMMUNICATIONS, 2007, 8 (03) :561-564

[3] STABILIZATION OF ALUMINAS BY RARE-EARTH AND ALKALINE-EARTH IONS [J].

CHURCH, JS ;

CANT, NW ;

TRIMM, DL .

APPLIED CATALYSIS A-GENERAL, 1993, 101 (01) :105-116

[4] A STUDY OF CARBON DEPOSITION ON CATALYSTS DURING THE PARTIAL OXIDATION OF METHANE TO SYNTHESIS GAS [J].

CLARIDGE, JB ;

GREEN, MLH ;

TSANG, SC ;

YORK, APE ;

ASHCROFT, AT ;

BATTLE, PD .

CATALYSIS LETTERS, 1993, 22 (04) :299-305

[5] Partial oxidation of n-hexadecane at short contact times:: Catalyst and washcoat loading and catalyst morphology [J].

Degenstein, N. J. ;

Subramanian, R. ;

Schmidt, L. D. .

APPLIED CATALYSIS A-GENERAL, 2006, 305 (02) :146-159

[6] SULFUR POISONING, RECOVERY AND RELATED PHENOMENA OVER SUPPORTED PALLADIUM, RHODIUM AND IRIDIUM CATALYSTS FOR METHANE OXIDATION [J].

DENG, YQ ;

NEVELL, TG ;

EWEN, RJ ;

HONEYBOURNE, CL ;

JONES, MG .

APPLIED CATALYSIS A-GENERAL, 1993, 101 (01) :51-62

[7]

FISHER GB, 2007, N AM CAT SOC 20 N AM

[8]

GOODMAN DW, 1984, P 2 S IND U COOP CHE, P230

[9]

Hedge R. I., 1986, J PHYS CHEM-US, V90, P296

[10] PRODUCTION OF SYNGAS BY DIRECT CATALYTIC-OXIDATION OF METHANE [J].

HICKMAN, DA ;

SCHMIDT, LD .

SCIENCE, 1993, 259 (5093) :343-346

← 1 2 3 →