TY  - JOUR
AU  - Solymosi, Thomas
AU  - Geißelbrecht, Michael
AU  - Mayer, Sophie
AU  - Auer, Michael
AU  - Leicht, Peter
AU  - Terlinden, Markus
AU  - Malgaretti, Paolo
AU  - Bösmann, Andreas
AU  - Preuster, Patrick
AU  - Harting, Jens
AU  - Thommes, Matthias
AU  - Vogel, Nicolas
AU  - Wasserscheid, Peter
TI  - Nucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems
JO  - Science advances
VL  - 8
IS  - 46
SN  - 2375-2548
CY  - Washington, DC [u.a.]
PB  - Assoc.
M1  - FZJ-2022-03731
SP  - eade3262
PY  - 2022
AB  - 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.
LB  - PUB:(DE-HGF)16
C6  - 36383668
UR  - <Go to ISI:>//WOS:000968029000001
DO  - DOI:10.1126/sciadv.ade3262
UR  - https://juser.fz-juelich.de/record/910296
ER  -