在Ru/CeO2催化剂上对CO2甲的活性场所依赖反应机制
Fei Wang1, Shan He1, Hao Chen1
1State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology , Beijing 100029, P. R. China.
Journal of the American Chemical Society
|May 3, 2016
概括
(CeO2) 中的氧气空缺是二氧化碳甲化的关键活性场所,促进了酸盐的形成,降低了决定速度的步骤.
科学领域:
- 不同质的催化
- 表面科学
- 材料化学
背景情况:
- 氧气空隙是金属氧化物表面的关键缺陷,在催化过程中充当反应点.
- 了解活性位点的作用对于优化CO2甲化等催化反应至关重要.
研究的目的:
- 对Ru/CeO2和Ru/α-Al2O3催化剂的二氧化碳甲化活动依赖地点的机制进行研究.
- 通过操作光谱学阐明催化过程中CeO2中氧气空缺的作用.
主要方法:
- 使用XANES,IR和拉曼光谱来研究反应条件下的催化剂演变.
- 在现场DRIFT红外光谱与稳态同位素瞬态动力分析 (SSITKA) 确定反应途径.
- 催化活性评估和振荡反应分析.
主要成果:
- 有氧空缺的Ru/CeO2通过甲酸盐路径促进CO2甲化,甲酸盐解离是决定速度的步骤.
- 没有氧气空缺的Ru/α-Al2O3通过Ru表面的CO路径促进CO2甲化.
- 氧气空位显著降低了速率决定阶段的激活温度 (125°C与250°C相比).
结论:
- 二氧化碳甲化的催化机制取决于活性部位,特别是氧气空缺的存在或不存在.
- 在CeO2中空缺的氧气作为关键的催化场所,在较低的温度下提高CO2转化效率.
- 这项研究提供了对二氧化碳甲化中的活性位点依赖反应机制的彻底了解.
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