Unravelling the Different Reaction Pathways for Low Temperature CO Oxidation on Pt/CeO2 and Pt/Al2O3 by Spatially Resolved Structure-Activity Correlations.,The Journal of Physical Chemistry Letters

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Unravelling the Different Reaction Pathways for Low Temperature CO Oxidation on Pt/CeO2 and Pt/Al2O3 by Spatially Resolved Structure-Activity Correlations.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2019-12-02 , DOI: 10.1021/acs.jpclett.9b02768
Andreas M Gänzler ₁ , Maria Casapu ₁ , Dmitry E Doronkin _{1,

2} , Florian Maurer ₁ , Patrick Lott ₁ , Pieter Glatzel ₃ , Martin Votsmeier ₄ , Olaf Deutschmann _{1,

2} , Jan-Dierk Grunwaldt _{1,

2}

Affiliation

Spatially resolved operando HERFD-XANES (high energy resolution fluorescence detected X-ray absorption near edge structure) complemented by CO concentration gradient profiles along the catalyst bed (SpaciPro) was used to identify the dominant reaction paths for the low and high temperature CO oxidation on Pt/CeO2 and Pt/Al2O3. At low temperatures, features associated with CO adsorption on Pt were found for both catalysts. During the oxidation reaction light-off, the evolution of the spectral and catalytic profile diverged along the catalyst bed. The CO oxidation rate was high on Pt/CeO2 from the beginning of the catalyst bed with CO being adsorbed on Pt, whereas low CO conversion due to strong CO poisoning was found on Pt/Al2O3. This correlation of the CO concentration gradient with unique insight by HERFD-XANES gave direct proof of the crucial contribution of the Pt-CeO2 perimeter sites overcoming the CO self-inhibition effect at low temperatures.

中文翻译：

通过空间解析的结构活性相关性揭示了Pt / CeO2和Pt / Al2O3上低温CO氧化的不同反应途径。

空间分辨操作HERFD-XANES（高能分辨率荧光检测到的X射线在边缘结构附近的吸收）与沿着催化剂床层的CO浓度梯度分布（SpaciPro）相辅相成，用于确定低温和高温下CO氧化的主要反应路径。 Pt / CeO2和Pt / Al2O3。在低温下，两种催化剂均发现与CO在Pt上吸附有关的特征。在氧化反应起燃期间，光谱和催化分布的演变沿催化剂床发散。从催化剂床层开始，Pt / CeO2上的CO氧化速率就很高，CO吸附在Pt上，而由于Pt / Al2O3上强烈的CO中毒，导致CO转化率低。

更新日期：2019-12-03

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