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@ARTICLE{Solymosi:910296,
author = {Solymosi, Thomas and Geißelbrecht, Michael and Mayer,
Sophie and Auer, Michael and Leicht, Peter and Terlinden,
Markus and Malgaretti, Paolo and Bösmann, Andreas and
Preuster, Patrick and Harting, Jens and Thommes, Matthias
and Vogel, Nicolas and Wasserscheid, Peter},
title = {{N}ucleation as a rate-determining step in catalytic gas
generation reactions from liquid phase systems},
journal = {Science advances},
volume = {8},
number = {46},
issn = {2375-2548},
address = {Washington, DC [u.a.]},
publisher = {Assoc.},
reportid = {FZJ-2022-03731},
pages = {eade3262},
year = {2022},
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.},
cin = {IEK-11},
ddc = {500},
cid = {I:(DE-Juel1)IEK-11-20140314},
pnm = {1232 - Power-based Fuels and Chemicals (POF4-123) / 1215 -
Simulations, Theory, Optics, and Analytics (STOA) (POF4-121)
/ DFG project 431791331 - SFB 1452: Katalyse an flüssigen
Grenzflächen},
pid = {G:(DE-HGF)POF4-1232 / G:(DE-HGF)POF4-1215 /
G:(GEPRIS)431791331},
typ = {PUB:(DE-HGF)16},
pubmed = {36383668},
UT = {WOS:000968029000001},
doi = {10.1126/sciadv.ade3262},
url = {https://juser.fz-juelich.de/record/910296},
}