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Comparison study of the effect of CeO2-based carrier materials on the total oxidation of CO, methane, and propane over RuO2
Catalysis Science & Technology ( IF 5 ) Pub Date : 2021-08-27 , DOI: 10.1039/d1cy01277k
Zheng Wang 1, 2 , Omeir Khalid 2 , Wei Wang 1, 2 , Yu Wang 1 , Tim Weber 2 , Alexander Spriewald Luciano 2 , Wangcheng Zhan 1 , Bernd M. Smarsly 2 , Herbert Over 2
Affiliation  

The effect of the carrier material on the intrinsic activity of three catalytic total oxidation reactions, namely CO oxidation and methane and propane combustion, over highly dispersed RuO2 is studied. The carrier materials are systematically varied from ZrO2 to CeO2 using ultrathin CeO2 films on ZrO2 particles (CeO2@ZrO2) as the linking carrier materials that were subjected to different calcination and redox treatments. CeO2@ZrO2 is subjected to annealing to 900 °C, transforming the CeO2 layer into a mixed CexZr1−xO2 layer, and finally, after reductive treatment with H2 at 950 °C and mild re-oxidation at 500 °C a kappa phase layer is formed on the ZrO2 core. The catalytic CO oxidation and the propane combustion reveal pronounced dependencies on the carrier material. The variation in propane combustion activity with the carrier material is correlated with the varying surface concentration of vacant surface Ce sites, while the activity in CO oxidation is correlated with the oxygen storage capacity (OSC). Quite in contrast, the intrinsic activity and the apparent activation energy in methane combustion are less affected by the carrier material than in the other two reactions. For comparison we chose rutile TiO2 as the carrier that is known to disperse RuO2 quite efficiently, revealing, however, by far the lowest activity in all total oxidation reactions studied, due likely to strong metal–support interaction (SMSI).

中文翻译:

CeO2基载体材料对RuO2上CO、甲烷和丙烷的总氧化影响的比较研究

研究了载体材料对高度分散的 RuO 2上三种催化总氧化反应(即 CO 氧化和甲烷和丙烷燃烧)的固有活性的影响。载体材料从 ZrO 2到 CeO 2系统地变化,使用ZrO 2颗粒上的超薄 CeO 2薄膜(CeO 2 @ZrO 2)作为连接载体材料,这些材料经过不同的煅烧和氧化还原处理。CeO 2 @ZrO 2退火至 900 °C,将 CeO 2层转变为混合的 Ce x Zr 1− x O2层,最后,在 950 °C 下用 H 2还原处理并在 500 °C 下温和再氧化后,在 ZrO 2核上形成 kappa 相层。催化 CO 氧化和丙烷燃烧揭示了对载体材料的显着依赖性。丙烷燃烧活性随载体材料的变化与空置表面 Ce 位点的表面浓度变化有关,而 CO 氧化活性与储氧能力 (OSC) 相关。相比之下,与其他两个反应相比,甲烷燃烧中的固有活性和表观活化能受载体材料的影响较小。为了比较,我们选择金红石 TiO 2作为已知分散 RuO 的载体2非常有效,然而,揭示了迄今为止研究的所有总氧化反应中最低的活性,这可能是由于强金属 - 载体相互作用(SMSI)。
更新日期:2021-09-15
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