%0 Journal Article
%A Solymosi, Thomas
%A Geißelbrecht, Michael
%A Mayer, Sophie
%A Auer, Michael
%A Leicht, Peter
%A Terlinden, Markus
%A Malgaretti, Paolo
%A Bösmann, Andreas
%A Preuster, Patrick
%A Harting, Jens
%A Thommes, Matthias
%A Vogel, Nicolas
%A Wasserscheid, Peter
%T Nucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems
%J Science advances
%V 8
%N 46
%@ 2375-2548
%C Washington, DC [u.a.]
%I Assoc.
%M FZJ-2022-03731
%P eade3262
%D 2022
%X 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%$ 36383668
%U <Go to ISI:>//WOS:000968029000001
%R 10.1126/sciadv.ade3262
%U https://juser.fz-juelich.de/record/910296