Activation mechanism of methane-derived coke (CHx) by CO2 during dry reforming of methane -: comparison for Pt/Al2O3 and Pt/ZrO2

被引:59
作者
Nagaoka, K
Seshan, K
Lercher, JA
Aika, K
机构
[1] Tokyo Inst Technol, Interdisciplinary Grad Sch Sci & Engn, Dept Environm Chem & Engn, Midori Ku, Yokohama, Kanagawa 2268502, Japan
[2] Univ Twente, Fac Chem Technol, NL-7500 AE Enschede, Netherlands
[3] Tech Univ Munich, Dept Phys Chem, D-85748 Garching, Germany
关键词
CH4/CO2; reforming; supported Pt catalysts; reactivity of coke with CO2; reactivity of coke itself; reactivity of CO2; oxygen defect site;
D O I
10.1023/A:1018877032022
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 reaction of methane-derived coke (CHx: intermediate of the reforming reaction and also a source of coke deposition) with CO2 was studied on supported Pt catalysts in relation with CO2 reforming of methane. Temperature-programmed hydrogenation (TPH) was performed to investigate the reactivity of coke deposition after the catalyst was exposed to CH4/He at 1070 K. Coke on Pt/Al2O3 could be hydrogenated around 873 K, while for Pt/ZrO2 this was above 1073 K. The results indicate that the reactivity of coke with hydrogen was higher on Pt/Al2O3 than on Pt/ZrO2, which was different from the reactivity of coke towards CO2. Thus, the reactivity of CO2 was studied and compared on these catalysts by several technics. The amount of CO evolution was measured during CO2 flow at 1070 and 875 K. Rate and amount of converted CO2 were higher on Pt/ZrO2 than on Pt/Al2O3. Pt/ZrO2 was proven to react with CO2 to produce CO and active oxygen (CO2 --> CO + O) (probably on its oxygen defect site) more easily than Pt/Al2O3.
引用
收藏
页码:109 / 116
页数:8
相关论文
共 24 条
[1]   IR SPECTROSCOPY OF (CO2)-O-18 ON ALUMINA/UMINA [J].
AMENOMIYA, Y ;
MORIKAWA, Y ;
PLEIZIER, G .
JOURNAL OF CATALYSIS, 1977, 46 (03) :431-433
[2]   PARTIAL OXIDATION OF METHANE TO SYNTHESIS GAS-USING CARBON-DIOXIDE [J].
ASHCROFT, AT ;
CHEETHAM, AK ;
GREEN, MLH ;
VERNON, PDF .
NATURE, 1991, 352 (6332) :225-226
[3]   Mono and bifunctional pathways of CO2/CH4 reforming over Pt and Rh based catalysts [J].
Bitter, JH ;
Seshan, K ;
Lercher, JA .
JOURNAL OF CATALYSIS, 1998, 176 (01) :93-101
[4]   Deactivation and coke accumulation during CO2/CH4 reforming over Pt catalysts [J].
Bitter, JH ;
Seshan, K ;
Lercher, JA .
JOURNAL OF CATALYSIS, 1999, 183 (02) :336-343
[5]   On the contribution of X-ray absorption spectroscopy to explore structure and activity relations of Pt/ZrO2 catalysts for CO2/CH4 reforming [J].
Bitter, JH ;
Seshan, K ;
Lercher, JA .
TOPICS IN CATALYSIS, 2000, 10 (3-4) :295-305
[6]   ACTIVATION OF CH4 AND ITS REACTION WITH CO2 OVER SUPPORTED RH CATALYSTS [J].
ERDOHELYI, A ;
CSERENYI, J ;
SOLYMOSI, F .
JOURNAL OF CATALYSIS, 1993, 141 (01) :287-299
[7]  
FOGER K, 1974, CATALYSIS SCI TECHNO, V6
[8]   HYDROCARBON FORMATION FROM METHANE BY A LOW-TEMPERATURE 2-STEP REACTION SEQUENCE [J].
KOERTS, T ;
DEELEN, MJAG ;
VANSANTEN, RA .
JOURNAL OF CATALYSIS, 1992, 138 (01) :101-114
[9]   INFRARED STUDIES OF ADSORBED SPECIES OF H-2, CO AND CO2 OVER ZRO2 [J].
KONDO, J ;
ABE, H ;
SAKATA, Y ;
MARUYA, K ;
DOMEN, K ;
ONISHI, T .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1988, 84 :511-519
[10]  
NAGAOKA K, UNPUB J CATAL