Journal Article

FZJ-2022-03731

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Nucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems

Solymosi, T.FZJ* ; Geißelbrecht, M.FZJ* ; Mayer, S. ; Auer, M. ; Leicht, P. ; Terlinden, M. ; Malgaretti, P.FZJ* ; Bösmann, A. ; Preuster, P.FZJ* ; Harting, J.FZJ* ; Thommes, M. ; Vogel, N. ; Wasserscheid, P. (Corresponding author)FZJ*

2022
Assoc. Washington, DC [u.a.]

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Please use a persistent id in citations: http://hdl.handle.net/2128/33964  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.

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Contributing Institute(s):

1. Helmholtz-Institut Erlangen-Nürnberg Erneuerbare Energien (IEK-11)

Research Program(s):

1. 1232 - Power-based Fuels and Chemicals (POF4-123) (POF4-123)
2. 1215 - Simulations, Theory, Optics, and Analytics (STOA) (POF4-121) (POF4-121)
3. DFG project 431791331 - SFB 1452: Katalyse an flüssigen Grenzflächen (431791331)

Appears in the scientific report 2022

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