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首页> 外文期刊>Catalysis Today >An operando DRIFTS-MS study on model Ce_(0.5)Zr_(0.5)O_2 redox catalyst:A critical evaluation of DRIFTS and MS data on CO abatement reaction
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An operando DRIFTS-MS study on model Ce_(0.5)Zr_(0.5)O_2 redox catalyst:A critical evaluation of DRIFTS and MS data on CO abatement reaction

机译：Ce_（0.5）Zr_（0.5）O_2氧化还原催化剂模型的DRIFTS-MS操作研究：DRIFTS和MS数据对减少CO反应的关键评估

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摘要

An operando study of CO oxidation by Ce_(0.5)Zr_(0.5)O_2 catalysts under dynamic conditions was performed using a prototype gas flow DRIFTS reaction chamber coupled with a MS.Previous studies conducted under oscillating CO/O_2 feedstream conditions,allowed the identification of carbonates as the C-containing storage species on the catalyst surface,with their decomposition being the origin of CO_2 evolution dynamics during O_2 pulses. A deeper comparison of the time-resolved DRIFTS and MS data revealed some differences that were related to the different observation points of the two detectors.Two methods for the determination of penetration depth of IR radiation in catalysts beds were compared and discussed.From the analysis of DRIFTS data,two main pathways for carbonates decomposition were found at the beginning of the bed of the catalysts:one leading to CO_2 and Ce(IV) sites and another to CO and Ce(III).The last one is active only above 673 K.The preference of one pathway against the other is strictly related to the Ce(III)/Ce(IV) ratio that shows strong variation during the entire cycle.
机译：使用原型气流DRIFTS反应室和MS进行了在动态条件下Ce_（0.5）Zr_（0.5）O_2催化剂对CO氧化的操作研究。以前的研究在振荡CO / O_2进料流条件下进行，从而确定了碳酸盐作为催化剂表面含C的存储物质，其分解是O_2脉冲过程中CO_2演化动力学的起源。对时间分辨的DRIFTS和MS数据进行了更深入的比较，发现了与两个探测器的不同观察点有关的一些差异。比较和讨论了两种确定催化剂床层IR辐射穿透深度的方法。从DRIFTS数据来看，在催化剂床层开始时发现了碳酸盐分解的两个主要途径：一个导致CO_2和Ce（IV）的位点，另一个导致CO和Ce（III）的位点。最后一个仅在673以上才有活性。 K.一种途径相对于另一种途径的偏好与Ce（III）/ Ce（IV）比率严格相关，后者在整个周期中显示出很大的变化。

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