Nature Catalysis ( IF 42.8 ) Pub Date : 2019-09-23 , DOI: 10.1038/s41929-019-0352-1 Thomas Hartman , Robin G. Geitenbeek , Gareth T. Whiting , Bert M. Weckhuysen
The development of improved catalysts requires insights into the relationship between catalytic activity and catalyst structure, including the underlying reaction mechanism. Here, we demonstrate a unique set of catalyst extrudate sensors that allow for the simultaneous detection of local temperature by luminescence thermometry, and of surface species by shell-isolated nanoparticle-enhanced Raman spectroscopy. This sensing approach was applied to the characterization of direct conversion of syngas into hydrocarbons and C2+ oxygenates over supported Rh and RhFe catalysts. Luminescence thermometry demonstrated a mismatch between the set temperature and the local catalyst temperature, with variations up to 40 °C. Furthermore, by investigating the surface species on varying extrudate and catalyst compositions, we identified tilted carbonyl species on the Rh/SiO2 interface that are probable precursors for the hydrogen-assisted CO dissociation. The implementation of extrudate catalyst sensors as a characterization tool provides a unique approach towards the further understanding of the relevant parameters in catalysis.
中文翻译:
在单个催化剂颗粒水平上对温度和活性物质进行操作监测
改进催化剂的开发需要深入了解催化活性与催化剂结构之间的关系,包括潜在的反应机理。在这里,我们演示了一套独特的催化剂挤出物传感器,该传感器可以通过发光测温法同时检测局部温度,并通过壳分离的纳米粒子增强拉曼光谱法同时检测表面物种。该感测方法用于表征合成气直接转化为碳氢化合物和C 2+的特征在负载型Rh和RhFe催化剂上氧化。发光测温法显示设定温度与局部催化剂温度之间不匹配,变化高达40°C。此外,通过研究不同挤出物和催化剂组成上的表面物质,我们在Rh / SiO 2界面上发现了倾斜的羰基物质,它们是氢辅助CO离解的可能前体。挤出物催化剂传感器作为表征工具的实施为进一步理解催化中的相关参数提供了一种独特的方法。