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The role of H2S addition on Pt/Al2O3 catalyzed propane dehydrogenation: a mechanistic study

机译:硫化氢的作用除了Pt /氧化铝催化丙烷脱氢:机械的研究

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摘要

Introducing sulfur species into Pt catalysts has been proven to be an effective method to improve their performance in various reactions. However, the role of sulfur addition on Pt catalysts catalyzing propane dehydrogenation (PDH) is still not clear. This work combines catalyst characterizations, catalytic kinetics studies and DFT calculations to understand the influence of H2S addition in the feed on Pt/-Al2O3 catalyzed PDH from a mechanistic perspective. With the addition of a trace amount of H2S in the feed (3 ppm), the propylene selectivity increases from 79% to 96% and the deactivation factor decreases from 33% to 18%, at the expense of a slight activity loss. The improved catalytic performance can be partially attributed to the electron transfer from sulfur species to Pt atoms as indicated by CO-DRIFTS results. DFT calculations show that H2S could be the dominating sulfur species on Pt particles and donate electrons to Pt atoms, which further proves that sulfur species improve the catalytic performance by donating electrons. In addition, the repulsion between sulfur species and C-3 hydrocarbons also explains the improved catalytic performance.
机译:将硫物种引入Pt催化剂被证明是一种有效的方法来改善他们的表现在不同的反应。硫对Pt添加催化剂的作用催化丙烷脱氢(PDH)仍然是不清楚。特征、催化动力学研究DFT计算理解的影响硫化氢在饲料添加Pt /氧化铝催化PDH从机械的角度来看。添加微量的硫化氢提要(3ppm),丙烯选择性增加和失活的因素减少79%至96%从33%提高到18%,以牺牲一个轻微的活动的损失。可以部分归因于电子从硫物种Pt原子转移由CO-DRIFTS表示结果。表明,硫化氢可以主导的硫物种Pt粒子和电子捐款Pt原子,这进一步证明了硫磺物种改善催化性能捐赠电子。硫物种之间和颈碳氢化合物解释了提高催化性能。

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