Dry reforming of methane over supported Rh and Ru catalysts: Effect of the support (Al2O3, TiO2, ZrO2, YSZ) on the activity and reaction pathway

被引：27
|
作者：
Androulakis, A. [1 ]
Yentekakis, I., V [1 ]
Panagiotopoulou, P. [1 ]
机构：
[1] Tech Univ Crete, Sch Chem & Environm Engn, Lab Environm Catalysis, GR-73100 Khania, Greece
来源：
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY | 2023年 / 48卷 / 87期
关键词：
Dry reforming of methane (DRM); H-2; productionRh; WATER-GAS SHIFT; METAL CRYSTALLITE SIZE; CARBON-DIOXIDE; MECHANISTIC ASPECTS; RU/TIO2; CATALYSTS; RHODIUM CATALYSTS; SYNGAS PRODUCTION; CO ADSORPTION; SELECTIVE METHANATION; NI;
D O I：
10.1016/j.ijhydene.2023.03.114
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 Al2O3, TiO2, ZrO2 and Yttria-Stabilized Zirconia (YSZ) supports on the activity of the dry reforming of CH4 towards syngas production was investigated for Rh and Ru catalysts. Ruthenium-based catalysts were found to generally be more active than Rh leading H-2/CO ratios close to unity above 700 degrees C. Methane conversion turnover frequency (TOF) over Rh catalysts becomes optimum for Rh/YSZ followed by Rh/TiO2 and Rh/ZrO2, and finally Rh/Al2O3, which exhibited the lowest activity. The performance order is different for Ru catalysts, with TOF being increased in the order Ru/Al2O3<Ru/TiO2<Ru/YSZ < Ru/ZrO2. Time-on-stream (TOS) stability tests showed that Rh/ZrO2 is stable for 30 h, whereas Ru/ZrO2 exhibits a slight decrease of both reactants' conversions. DRIFTS studies indicated that the reaction proceeds via a bifunctional mechanism involving both the metal and the support in the reaction pathway. The population and adsorption sites of produced carbonyls are strongly influenced by the metal-support combination determining the catalytic activity.
引用
收藏
页码：33886 / 33902
页数：17
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