A combined in situ time-resolved UV-Vis, Raman and high-energy resolution X-ray absorption spectroscopy study on the deactivation behavior of Pt and Pt-Sn propane dehydrogenation catalysts under industrial reaction conditions
A combined in situ time-resolved UV-Vis, Raman and high-energy resolution X-ray absorption spectroscopy study on the deactivation behavior of Pt and Pt-Sn propane dehydrogenation catalysts under industrial reaction conditions
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DOI：
10.1016/j.jcat.2010.09.018
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发表时间：
2010-12-15
影响因子：
7.3
通讯作者：
Weckhuysen, Bert M.
中科院分区：
文献类型：
--
作者：
Iglesias-Juez, Ana;Beale, Andrew M.;Weckhuysen, Bert M.
在实际反应条件下，考察了铂/氧化铝和铂-锡/氧化铝催化剂在丙烷脱氢连续反应再生循环中的催化性能。为了考察催化剂的活性和稳定性，以及丙烯选择性，结合原位紫外可见/拉曼光谱测量，进行了与工业丙烷脱氢反应器相似的10次连续脱氢再生循环研究。为了跟踪丙烷脱氢过程中的结焦过程，该方法允许丙烷转化率和丙烯生成量与在线测定的拉曼D/G带强度比和结焦量相关联。在焦炭形成和相关催化剂失活的原位测量中，补充了原位高能分辨荧光检测(HERFD)XANES测量，以表征在连续的脱氢-再生循环中负载的铂和铂-锡纳米颗粒的结构和电子性质。这种强大的光谱技术的组合揭示了关于铂和铂-锡基丙烷脱氢催化剂的活性行为和失活机理的独特信息，使我们能够确定重要的结构-电子-性能关系以及对高温下纳米铂中铂-锡合金的形成过程的基本洞察(C)2010 Elsevier Inc.版权所有
The catalytic performances of Pt/Al2O3 and Pt-Sn/Al2O3 catalysts for the dehydrogenation of propane through consecutive reaction-regeneration cycles have been studied under realistic reaction conditions A 10-fold successive dehydrogenation-regeneration cycling study similar to that employed in an industrial propane dehydrogenation reactor was performed in order to examine the catalyst activity and stability as well as the propene selectivity Combined in situ UV-Vis/Raman spectroscopy measurements were taken in order to follow the coke formation processes during propane dehydrogenation This approach allowed correlating propane conversion and propene formation with the on-line determined Raman D over G band intensity ratio and amount of coke formed These in situ measurements on coke formation and related catalyst deactivation were supplemented by in situ high-energy resolution fluorescence detected (HERFD) XANES measurements in order to characterize the structural and electronic properties of the supported Pt and Pt-Sn nanoparticles during the successive dehydrogenation-regeneration cycles This combination of powerful spectroscopic techniques revealed unique information regarding the activity behavior and deactivation mechanism of Pt- and Pt-Sn-based propane dehydrogenation catalysts enabling us to identify Important structure-electronic-performance relationships as well as fundamental insight Into the dynamics of Pt-Sn alloy formation processes in Pt nanoparticles at elevated temperatures (C) 2010 Elsevier Inc All rights reserved