Nucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems

Solymosi T, Geißelbrecht M, Mayer S, Auer M, Leicht P, Terlinden M, Malgaretti P, Bösmann A, Preuster P, Harting J, Thommes M, Vogel N, Wasserscheid P (2022)

Publication Language: English

Publication Status: Published

Publication Type: Journal article

Publication year: 2022

Journal

Science Advances American Association for the Advancement of Science

Book Volume: 8

Journal Issue: 46

DOI: 10.1126/sciadv.ade3262

Abstract

The observable reaction rate of heterogeneously catalyzed reactions is known to be limited either by the intrinsic kinetics of the catalytic transformation or by the rate of pore and/or film diffusion. Here, we show that in gas generation reactions from liquid reactants, the nucleation of gas bubbles in the catalyst pore structure represents an additional important rate-limiting step. This is highlighted for the example of catalytic hydrogen release from the liquid organic hydrogen carrier compound perhydro-dibenzyltoluene. A nucleation-inhibited catalytic system produces only dissolved hydrogen with fast saturation of the fluid phase around the active site, while bubble formation enhances mass transfer by more than a factor of 50 in an oscillating reaction regime. Nucleation can be efficiently triggered not only by temperature changes and catalyst surface modification but also by a mechanical stimulus. Our work sheds new light on performance-limiting factors in reactions that are of highest relevance for the future green hydrogen economy.

Authors with CRIS profile

Sophie Mayer Professur für Partikelsynthese Peter Leicht Lehrstuhl für Thermische Verfahrenstechnik (TVT) Markus Terlinden Lehrstuhl für Thermische Verfahrenstechnik (TVT) Andreas Bösmann Lehrstuhl für Chemische Reaktionstechnik (CRT) Matthias Thommes Lehrstuhl für Thermische Verfahrenstechnik (TVT) Nicolas Vogel Professur für Partikelsynthese Peter Wasserscheid Lehrstuhl für Chemische Reaktionstechnik (CRT)

Related research project(s)

Support design for enhanced catalytic activity of SILP systems (B03) (SFB 1452 CLINT B03) Catalysis at Liquid Interfaces (CLINT) (SFB 1452 CLINT) Jan. 1, 2021 - Dec. 31, 2024

Involved external institutions

Forschungszentrum Jülich / Research Centre Jülich (FZJ) DE Germany (DE)

How to cite

APA:

Solymosi, T., Geißelbrecht, M., Mayer, S., Auer, M., Leicht, P., Terlinden, M.,... Wasserscheid, P. (2022). Nucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems. Science Advances, 8(46). https://doi.org/10.1126/sciadv.ade3262

MLA:

Solymosi, Thomas, et al. "Nucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems." Science Advances 8.46 (2022).

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