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

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• 作者：Joan Papavasiliou ; George Avgouropoulos ; Theophilos Ioannides
• 关键词：SSITKA ; Steam reforming ; Methanol ; Copper ; Ceria ; Manganese
• 刊名：Applied Catalysis B: Environmental
• 出版年：2009
• 出版时间：20 May 2009
• 年：2009
• 卷：88
• 期：3-4
• 页码：490-496
• 全文大小：614 K

文摘

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: ¹²CH₃OH/H₂O/Ar/He → ¹³CH₃OH/H₂O/He and CH₃OH/H₂¹⁶O/Ar/He → CH₃OH/H₂¹⁶O/H₂¹⁸O/He. The presence of CH₃¹⁸OH in the products after the switch to ¹⁸O-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.