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

页码：33886 / 33902

页数：17

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