Mass transfer considerations for monitoring catalytic solid–liquid interfaces under operating conditions,Reaction Chemistry & Engineering

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Mass transfer considerations for monitoring catalytic solid–liquid interfaces under operating conditions
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2017-12-18 00:00:00 , DOI: 10.1039/c7re00179g
Laura Rodríguez-García _{1,

2,

3,

4,

5} , Roland Walker _{1,

2,

3,

4,

5} , Eyal Spier _{5,

6,

7} , Konrad Hungerbühler _{1,

2,

3,

4,

5} , Fabian Meemken _{1,

2,

3,

4,

5}

Affiliation

Correlating catalytic performance and molecular-level information from the same catalyst sample is a promising approach to cope with the complexity of multiphase catalytic systems and to provide detailed mechanistic insight. To obtain information about the intrinsic reaction kinetics, the development of operando spectroscopy requires operation as well as surface-sensitive detection of the catalytic process in the absence of mass transfer limitations. In the present work, we investigated the effect of mass transfer on the detection of active species at the catalytic solid–liquid interface using attenuated total reflection-infrared (ATR-IR) spectroscopy. To gain a profound understanding of the mass transport within typical flow-through cells we have assessed the hydrodynamics as well as the transport of solutes within the liquid phase and the porous catalyst sample using a convection–diffusion model. The combination of computational and experimental data revealed four sensitive design parameters controlling the mass transfer within the ATR-IR spectroscopy cells. Using the asymmetric hydrogenation of phenyl cinnamic acid on a chirally modified Pd catalyst as a model reaction, we demonstrate the effects of mass transfer within the catalyst sample on the activity and selectivity.

中文翻译：

在操作条件下监测催化固液界面的传质注意事项

关联来自同一催化剂样品的催化性能和分子水平信息是一种有前途的方法，可以应对多相催化系统的复杂性并提供详细的机理信息。为了获得有关内在反应动力学，操作学发展的信息在没有传质限制的情况下，光谱学需要对催化过程进行操作以及表面敏感的检测。在当前的工作中，我们使用衰减全反射红外（ATR-IR）光谱技术研究了传质对催化固液界面活性物种检测的影响。为了深入了解典型流通池中的质量传递，我们使用对流扩散模型评估了流体动力学以及液相和多孔催化剂样品中溶质的传递。计算和实验数据的组合揭示了四个敏感的设计参数，这些参数控制着ATR-IR光谱仪内的传质。

更新日期：2017-12-18

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