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Insights into the CO2 deoxygenation to CO over oxygen vacancies of CeO2

机译:洞察二氧化碳脱氧作用有限氧气CeO2的空缺

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Cerium oxide (CeO2) is known to exhibit oxygen vacancy enhanced catalytic activity by itself or as a support. The particle shape effect on CO or VOC oxidation is also documented. This study reports the CO2 deoxygenation to CO over oxygen vacancies of CeO2 of different shapes, which can be a viable approach for CO2 utilization. A sequential experimental approach using a combination of TPR (temperature-programmed reduction under H-2 up to 900 degrees C), TPO (temperature-programmed oxidation under 20% O-2 up to 900 degrees C), and CO2 pulse reaction is performed. Tube and polyhedra CeO2 exhibit shape stability after TPR while cube and rod turn into polyhedral grains. Within a TPR-TPO-TPR or a TPR-CO2-TPR-CO2 test sequence, the tube sample shows the best reversibility in oxygen vacancy formation (based on the H-2 consumption ratio in the two TPRs) and the highest oxygen vacancy capacity (based on the second TPR) among the four samples. The CO2 deoxygenation to CO occurs over the four TPR-treated samples and the initial per pulse CO2 conversion is steady, implying that the surface reaction governs the rate and that the diffusion of stripped oxygen into the bulk phase is relatively fast. The deoxygenation reactivity is reproducible in the two CO2 pulsing tests in TPR-CO2-TPR-CO2 experiments, indicating the importance of reversibly generated oxygen vacancies. The results also indicate that the deoxygenation activity of surface oxygen vacancies can be influenced by subsurface vacancies.
机译:氧化铈(CeO2)表现出氧气空置本身或增强的催化活性作为支持。挥发性有机化合物氧化也记录。报告的二氧化碳脱氧对氧气有限公司职位空缺CeO2的不同形状,可以二氧化碳的利用是一种可行的方法。使用一个连续的实验方法TPR(程序升温的组合减少在2到900摄氏度),传真照片(程序升温氧化0 2 20%900摄氏度),二氧化碳脉冲反应执行。TPR而立方体和杆变成后稳定多面体的谷物。TPR-CO2-TPR-CO2测试序列,管样品展示最好的可逆性氧空位形成(基于2消费比例两个tpr)和最高的氧空位能力(基于第二个TPR)四种样本。四个TPR-treated和最初的样品脉冲二氧化碳转换是稳定的,这意味着管理的速度和表面反应剥夺了氧气扩散进入体相相对比较快。两个二氧化碳可再生的脉冲测试吗TPR-CO2-TPR-CO2实验,表明可逆地生成氧气的重要性职位空缺。脱氧活性表面的氧气可以受到地下空缺职位空缺。

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