Steady-state isotopic transient kinetic analysis of steam reforming of methanol over Cu-based catalysts

被引：60

作者：

Papavasiliou, Joan ^{[1
,2
]}

Avgouropoulos, George ^{[1
]}

Ioannides, Theophilos ^{[1
]}

机构：

[1] Inst Chem Engn & High Temp Chem Proc ICE HT, Fdn Res & Technol Hellas FORTH, GR-26500 Patras, Greece

[2] Univ Patras, Dept Chem Engn, GR-26500 Patras, Greece

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2009年 / 88卷 / 3-4期

关键词：

SSITKA; Steam reforming; Methanol; Copper; Ceria; Manganese; CU/ZNO/AL2O3; CATALYST; MECHANISTIC ASPECTS; HYDROGEN; COPPER; WATER; MN; COMBUSTION; SSITKA; ZN;

D O I：

10.1016/j.apcatb.2008.10.018

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：

Mechanistic aspects of steam reforming of methanol were studied via steady-state isotopic transient kinetic analysis over three copper-based catalysts, namely combustion-synthesized Cu-Ce-O and Cu-Mn-O, and commercial Cu-ZnO-Al2O3. The "C-path" and "O-path" for the production of CO2 via steam reforming of methanol was analysed with the following step changes in the feed: (CH3OH)-C-12/H2O/Ar/He -> (CH3OH)-C-13/H2O/He and CH3OH/(H2O)-O-16/Ar/He -> CH3OH/(H2O)-O-16/(H2O)-O-18/He. The presence of (CH3OH)-O-18 in the products after the switch to O-18-labeled water indicates that a major path of the reaction is the one involving a methyl formate intermediate. This appears to be the main path over the Cu-Mn-O catalyst, while parallel paths via dioxomethylene and methyl formate intermediates appear to be operative over Cu-Ce-O and Cu-ZnO-Al2O3 catalysts. (C) 2008 Elsevier B.V. All rights reserved.

引用

页码：490 / 496

页数：7

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