Calcination temperature and CuO loading dependence on CuO-CeO2 catalyst activity for water-gas shift reaction
Calcination temperature and CuO loading dependence on CuO-CeO2 catalyst activity for water-gas shift reaction
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DOI：
10.1016/j.apcata.2008.05.027
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发表时间：
2008-09-01
影响因子：
5.5
通讯作者：
Pintar, Albin
中科院分区：
文献类型：
--
作者：
Djinovic, Petar;Batista, Jurka;Pintar, Albin
在这项工作中，我们研究了 CuO 负载和催化剂预处理程序的影响，以获得用于水煤气变换 (WGS) 反应的最佳 CuO-CeO2 催化剂，并详细研究了结构-活性关系。通过 XRD、BET 和 TPR/TPD 分析对通过共沉淀制备的 CuO 含量为 10、15 和 20 mol% 的纳米结构催化剂样品进行了检查，并在 180-400 摄氏度的温度范围内进行了脉冲 WGS 活性测试。通过 TPR/TPD 和 N2O 化学吸附分析进行了评估，随着 CuO 负载量的增加，细分散的 CuO 纳米粒子的部分代表较大的 CuO 聚集体而减少。所有催化剂样品在 WGS 反应中都观察到强烈的表面结构-活性依赖性。据证实，增加 CuO 含量会导致 CeO2 还原程度更高，这对 WGS 反应过程中 H-2 的生产产生积极影响。另一方面，提高煅烧温度会减少 BET 表面积，这是由 CuO 烧结和 CeO2 颗粒团聚引起的，从而对 H-2 生产产生负面影响。对于所有 CuO 负载量，观察到了独特的 WGS 活性对所检查固体表面酸度的依赖性。 ((c))2008 Elsevier B.V. 保留所有权利。
In this work we investigated the influence of CuO loading and catalyst pretreatment procedure to derive an optimal CuO-CeO2 catalyst for water-gas shift (WGS) reaction, and to study in detail structure-activity relationships. Nanostructured catalyst samples prepared by co-precipitation and a 10, 15 and 20 mol% CuO content were examined by XRD, BET and TPR/TPD analyses and subjected to pulse WGS activity tests in the temperature range of 180-400 degrees C. As evaluated by TPR/TPD and N2O chemisorption analyses, with increasing CuO loading the portion of finely dispersed CuO nanoparticles decreases on behalf of larger CuO aggregates. Strong surface structure-activity dependence in WGS reaction was observed for all catalyst samples. It was established that increasing CuO content results in higher extent of CeO2 reduction, which has a positive effect on H-2 Production during the WGS reaction. Increasing calcination temperature on the other hand reduces BET surface area, induced by CuO sintering and agglomeration of CeO2 particles resulting in a negative effect on H-2 production. Distinctive WGS activity dependence on surface acidity of examined solids was observed for all CuO loadings. ((c))2008 Elsevier B.V. All rights reserved.