Vogel Robin, Prins P Tim, Rabouw Freddy T, Weckhuysen Bert M
Inorganic Chemistry and Catalysis Group, Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science, Utrecht University Universiteitsweg 99 3584 CG Utrecht The Netherlands
Soft Condensed Matter Group, Debye Institute for Nanomaterials Science, Utrecht University Princetonplein 1 3584 CC Utrecht The Netherlands.
Catal Sci Technol. 2023 Sep 7;13(22):6366-6376. doi: 10.1039/d3cy00967j. eCollection 2023 Nov 13.
Raman spectroscopy is a powerful analytical tool to provide new insights in the working and deactivation principles of solid catalysts. Intense fluorescence can obscure Raman spectra to the extent that they become uninterpretable. Time-gated Raman spectroscopy, based on pulsed excitation and time-gated detection, suppresses background fluorescence based on its slower time dynamics compared to Raman scattering. In this work, we demonstrate and quantify the benefit of time gating for Raman spectroscopy, using the propane dehydrogenation reaction over Pt-Sn-based catalyst materials as a case study. Experimental time-gated Raman spectroscopy data are fitted to a time-trace model that is used to optimize time gating for the maximum signal-to-background-noise ratio. Time-gated Raman spectra of a spent propane dehydrogenation catalyst material show lower background fluorescence compared to the time-integrated Raman spectra counterparts. Simultaneous time-gated and time-integrated Raman spectroscopy experiments demonstrate the benefit of time gating to obtain more distinct Raman features, especially in the early coking stages where spectra are dominated by background fluorescence.
拉曼光谱是一种强大的分析工具，可在固体催化剂的工作和失活原理方面提供新的见解。强烈的荧光会使拉曼光谱变得模糊不清，以至于无法解读。基于脉冲激发和时间选通检测的时间选通拉曼光谱，与拉曼散射相比，基于其较慢的时间动态来抑制背景荧光。在这项工作中，我们以在Pt-Sn基催化剂材料上进行的丙烷脱氢反应为例，展示并量化了时间选通对拉曼光谱的益处。将实验时间选通拉曼光谱数据拟合到一个时间轨迹模型，该模型用于优化时间选通以获得最大的信背噪比。与时间积分拉曼光谱相比，废丙烷脱氢催化剂材料的时间选通拉曼光谱显示出更低的背景荧光。同时进行的时间选通和时间积分拉曼光谱实验证明了时间选通在获得更清晰的拉曼特征方面的益处，特别是在早期结焦阶段，此时光谱主要由背景荧光主导。
