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000910296 1001_ $$0P:(DE-Juel1)180742$$aSolymosi, Thomas$$b0
000910296 245__ $$aNucleation as a rate-determining step in catalytic gas generation reactions from liquid phase systems
000910296 260__ $$aWashington, DC [u.a.]$$bAssoc.$$c2022
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000910296 520__ $$aThe 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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000910296 7001_ $$0P:(DE-Juel1)180645$$aGeißelbrecht, Michael$$b1
000910296 7001_ $$0P:(DE-HGF)0$$aMayer, Sophie$$b2
000910296 7001_ $$0P:(DE-HGF)0$$aAuer, Michael$$b3
000910296 7001_ $$0P:(DE-HGF)0$$aLeicht, Peter$$b4
000910296 7001_ $$0P:(DE-HGF)0$$aTerlinden, Markus$$b5
000910296 7001_ $$0P:(DE-Juel1)185890$$aMalgaretti, Paolo$$b6
000910296 7001_ $$0P:(DE-HGF)0$$aBösmann, Andreas$$b7
000910296 7001_ $$0P:(DE-Juel1)174308$$aPreuster, Patrick$$b8
000910296 7001_ $$0P:(DE-Juel1)167472$$aHarting, Jens$$b9
000910296 7001_ $$0P:(DE-HGF)0$$aThommes, Matthias$$b10
000910296 7001_ $$0P:(DE-HGF)0$$aVogel, Nicolas$$b11
000910296 7001_ $$0P:(DE-Juel1)162305$$aWasserscheid, Peter$$b12$$eCorresponding author$$ufzj
000910296 773__ $$0PERI:(DE-600)2810933-8$$a10.1126/sciadv.ade3262$$gVol. 8, no. 46, p. eade3262$$n46$$peade3262$$tScience advances$$v8$$x2375-2548$$y2022
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