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100 1 _ |a Solymosi, Thomas
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245 _ _ |a Nucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems
260 _ _ |a Washington, DC [u.a.]
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520 _ _ |a 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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700 1 _ |a Mayer, Sophie
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700 1 _ |a Auer, Michael
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700 1 _ |a Leicht, Peter
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700 1 _ |a Terlinden, Markus
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700 1 _ |a Malgaretti, Paolo
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700 1 _ |a Bösmann, Andreas
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700 1 _ |a Harting, Jens
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700 1 _ |a Wasserscheid, Peter
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773 _ _ |a 10.1126/sciadv.ade3262
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