Hydrogen liberation from the hydrolytic dehydrogenation of dimethylamine-borane at room temperature by using a novel ruthenium nanocatalyst

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dc.contributor.authorCaliskan, Salim
dc.contributor.authorZahmakiran, Mehmet
dc.contributor.authorDurap, Feyyaz
dc.contributor.authorOzkar, Saim
dc.date.accessioned2024-04-24T16:24:05Z
dc.date.available2024-04-24T16:24:05Z
dc.date.issued2012
dc.departmentDicle Üniversitesien_US
dc.description.abstractHerein we report the discovery of an in situ generated, highly active nanocatalyst for the room temperature dehydrogenation of dimethylamine-borane in water. The new catalyst system consisting of ruthenium(0) nanoparticles stabilized by the hydrogenphosphate anion can readily and reproducibly be formed under in situ conditions from the dimethylamine-borane reduction of a ruthenium(III) precatalyst in tetrabutylammonium dihydrogenphosphate solution at 25 +/- 0.1 degrees C. These new water dispersible ruthenium nanoparticles were characterized by using a combination of advanced analytical techniques. The results show the formation of well-dispersed ruthenium(0) nanoparticles of 2.9 +/- 0.9 nm size stabilized by the hydrogenphosphate anion in aqueous solution. The resulting ruthenium(0) nanoparticles act as a highly active catalyst in the generation of 3.0 equiv. of H-2 from the hydrolytic dehydrogenation of dimethylamine-borane with an initial TOF value of 500 h(-1) at 25 +/- 0.1 degrees C. Moreover, they provide exceptional catalytic lifetime (TTO = 11 600) in the same reaction at room temperature. The work reported here also includes the following results; (i) monitoring the formation kinetics of the in situ generated ruthenium nanoparticles, by using the hydrogen generation from the hydrolytic dehydrogenation of dimethylamine-borane as a catalytic reporter reaction, shows that sigmoidal kinetics of catalyst formation and concomitant dehydrogenation fits well to the two-step, slow nucleation and then autocatalytic surface growth mechanism, A -> B (rate constant k(1)) and A + B -> 2B (rate constant k(2)), in which A is RuCl3 center dot 3H(2)O and B is the growing, catalytically active Ru(0)(n) nanoclusters. (ii) Hg(0) poisoning coupled with activity measurements after solution infiltration demonstrates that the in situ generated ruthenium(0) nanoparticles act as a kinetically competent heterogeneous catalyst in hydrogen generation from the hydrolytic dehydrogenation of dimethylamine-borane. (iii) A compilation of kinetic data depending on the temperature and catalyst concentration is used to determine the dependency of reaction rate on catalyst concentration and the activation energy of the reaction, respectively.en_US
dc.description.sponsorshipTurkish Academy of Sciencesen_US
dc.description.sponsorshipPartial support by Turkish Academy of Sciences is gratefully acknowledged.en_US
dc.identifier.doi10.1039/c2dt00042c
dc.identifier.endpage4984en_US
dc.identifier.issn1477-9226
dc.identifier.issn1477-9234
dc.identifier.issue16en_US
dc.identifier.pmid22410969
dc.identifier.scopus2-s2.0-84859259650
dc.identifier.scopusqualityQ2
dc.identifier.startpage4976en_US
dc.identifier.urihttps://doi.org/10.1039/c2dt00042c
dc.identifier.urihttps://hdl.handle.net/11468/16466
dc.identifier.volume41en_US
dc.identifier.wosWOS:000302023800035
dc.identifier.wosqualityQ1
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.indekslendigikaynakPubMed
dc.language.isoenen_US
dc.publisherRoyal Soc Chemistryen_US
dc.relation.ispartofDalton Transactions
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanıen_US
dc.rightsinfo:eu-repo/semantics/closedAccessen_US
dc.subject[No Keyword]en_US
dc.titleHydrogen liberation from the hydrolytic dehydrogenation of dimethylamine-borane at room temperature by using a novel ruthenium nanocatalysten_US
dc.titleHydrogen liberation from the hydrolytic dehydrogenation of dimethylamine-borane at room temperature by using a novel ruthenium nanocatalyst
dc.typeArticleen_US

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