4.7 Article

3D printed catalytic reactors for aerobic selective oxidation of benzyl alcohol into benzaldehyde in continuous multiphase flow

Journal

SUSTAINABLE MATERIALS AND TECHNOLOGIES
Volume 30, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.susmat.2021.e00329

Keywords

Continuous flow reactor; Heterogeneous catalysis; 3D printed catalysts; Benzyl alcohol oxidation; Alcohol aerobic oxidation

Funding

  1. VITO

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This study introduces novel patterned monolithic reactors as potential replacements for conventional packed bed and batch reactors in the chemical industry. By utilizing bimetallic formulations, including earth-abundant metals like iron, higher conversion rates and TOF values were achieved in the selective oxidation of benzyl alcohol. Mathematical modeling provided insights into the physical and chemical processes governing reactant conversion, highlighting the advantages of the novel design.
In this work, novel, patterned monolithic reactors were devised to explore more efficient routes for reactant conversion in order to investigate their potential to replace the packed bed and batch reactors conventionally employed in chemical industries. Well-defined bimetallic formulations were developed to substitute platinum group metals and critical raw materials such as palladium and cobalt, at least in part, by less active, but more sustainable and cost-effective metals such as earth-abundant iron. FePd and FeCo based monoliths were 3D printed and stacked in a continuous flow tubular reactor for testing the selective oxidation of benzyl alcohol (BA) into benzaldehyde (BZ) under mild conditions (80-100 degrees C and atmospheric pressure). The novel monolithic reactors were evaluated against current state-of-the-art reactor technologies, conventional packed bed and batch reactors. The FeCo- and FePd-Al2O3-supported monolithic catalyst beds showed higher conversion and TOF than their packed bed counterparts under the same operating conditions, revealing the impact of the novel design on both regular geometry and composition. What is of particular interest in the catalytic measurements shown is that the combined stacking of two monoliths in a flow reactor, Al2O3-supported Fe and GO-supported FePd catalysts, can significantly improve the performance with an increase in TOF of up to 90% in comparison to their FePd analogues. Mathematical modelling was used to obtain additional insights into the physical and chemical processes governing the rate of BA conversion. It was found that due to the flow regime inside the microchannels, an axial dispersion model was appropriate, which allowed for mapping the concentration profiles of the reactants and products within the respective monolith geometries.

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