烃类转化催化的发光测温:处理催化剂光学性质的动态变化

IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Robin Vogel, Daniël W. Groefsema, Maria A. van den Bulk, Thimo S. Jacobs, P. Tim Prins, Freddy T. Rabouw and Bert M. Weckhuysen*, 
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引用次数: 0

摘要

发光测温为催化过程的温度传感提供了一种有吸引力的策略,即嵌入在反应器中的荧光粉材料的温度依赖性发光被远程激发和记录。然而,催化剂材料光学性质的变化会扭曲发光记录,导致温度传感不准确。这在碳氢化合物转化催化中尤其成问题,因为碳沉积物的积累会使材料着色,并在激发时产生荧光。在这项工作中,我们开发了operando反射校正时间门控发光测温法,使用高动态和工业相关的pt - sn基丙烷脱氢(PDH)催化剂和Eu3+基荧光粉作为展示。PDH催化剂材料通过碳的沉积失活,随后通过氧化再生处理去除碳。在这些交替的反应-再生过程中,催化剂材料的背景荧光和颜色不断变化。这会扭曲Eu3+的发光,导致温度读出伪影。我们通过脉冲激发后的时间门通检测来拒绝背景荧光,并通过校正PDH催化剂的波长依赖性吸收变化来解决这些问题。该方法提供了PDH催化剂材料的精确温度传感,并且在具有高动态光学性质的样品的发光测温发展中向前迈出了一步。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Operando Luminescence Thermometry for Hydrocarbon Conversion Catalysis: Dealing with Dynamic Changes in Catalyst Optical Properties

Luminescence thermometry offers an attractive strategy for temperature sensing of a catalytic process, whereby the temperature-dependent luminescence of a phosphor material embedded in the reactor is excited and recorded remotely. However, changes in the optical properties of the catalyst materials can distort the luminescence recording, resulting in inaccurate temperature sensing. This is particularly problematic in hydrocarbon conversion catalysis due to the buildup of carbon deposits, which color the material and cause fluorescence upon excitation. In this work, we developed operando reflectance-corrected time-gated luminescence thermometry, using a highly dynamic and industrially relevant Pt–Sn-based propane dehydrogenation (PDH) catalyst and an Eu3+-based phosphor as a showcase. PDH catalyst materials deactivate via the deposition of carbon, which is subsequently removed by an oxidative regeneration treatment. During these alternating reaction–regeneration processes, the background fluorescence and the color of the catalyst material change continuously. This skews the Eu3+ luminescence, leading to temperature-readout artifacts. We solved these problems by rejecting background fluorescence using time-gated detection following pulsed excitation and by correcting for the wavelength-dependent absorption changes of the PDH catalyst. This method offers accurate temperature sensing of the PDH catalyst material and is a step forward in the development of luminescence thermometry for samples with highly dynamic optical properties.

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来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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