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TEGTIC

Thermal effects on gas transport in catalytic membrane reactors
Funder: French National Research Agency (ANR)Project code: ANR-23-CE51-0055
Funder Contribution: 291,473 EUR
Description

Macroscale diffusion effects are well described by Navier-Stokes equations. In meso- and micropores, however, wall effects control gas flows and thus often catalytic reactions. Under dilute conditions, additional mass transport effects occur (thermal creep, Soret and Dufour effects) which are summarized as temperature-driven mass flow (TDF). TDF, which increases with temperature gradient may have a significant impact on catalytic reactions. These differences are determined by several parameters, (heat of reaction, thermal conductivity and dimensions). However, in reactor models, TDF was ignored or, in rare cases neglected. There is no empirical study showing quantification of TDF for catalytic reactions. We aim to fill this gap and evaluate conditions requiring TDF model use for exothermic reactions such as hydrogenations. It will be shown whether TDF can improve the model predictions, and whether mass transfer limitations in catalytic reactors can be reduced by superimposed TDF. We aim to establish a model building block for the assignment of thermal transport effects based on a scale bridging of TDF effects from the mesopore level macropore and from pore level to bulk flow. To relate thermal effects to structural and physical properties, experimental studies start with single channels, progress to multiple parallel ones (geometrically well-defined membrane), and to mesoporous membranes for catalytic reactions. As complexity increases, the individual contributions of thermal effects can be gradually revealed. TDF effects will be studied in individual channels and transferred to parallelized channel networks and mesoporous membranes impregnated with a Pt catalyst and used for hydrogenation reactions, accompanied by operando NMR measurements of concentration and temperature profiles. These non-invasive reactor- scale measurements will be used to cross-validate simulations of the effects of thermally induced mass transport in porous materials on catalytic reactions.

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