Hydroxyapatite-Nanosphere Supported Ruthenium(0) Nanoparticle Catalyst for Hydrogen Generation From Ammonia-Borane Solution: Kinetic Studies for Nanoparticle Formation and Hydrogen Evolution

dc.authorid Ozkar, S/0000-0002-6302-1429
dc.authorid Kaya, Murat/0000-0002-2458-8924
dc.authorid Gulcan, Mehmet/0000-0002-3921-8811
dc.authorscopusid 8854237200
dc.authorscopusid 8226754300
dc.authorscopusid 14521641300
dc.authorscopusid 7003408746
dc.authorscopusid 57206407342
dc.authorwosid Ozkar, S/ABA-1983-2020
dc.authorwosid Zahmakiran, Mehmet/F-7120-2014
dc.authorwosid Gülcan, Mehmet/HTP-5527-2023
dc.authorwosid Gülcan, Mehmet/AAT-1504-2021
dc.authorwosid Durak, Halil/I-8841-2019
dc.contributor.author Durak, Halil
dc.contributor.author Gulcan, Mehmet
dc.contributor.author Zahmakiran, Mehmet
dc.contributor.author Ozkar, Saim
dc.contributor.author Kaya, Murat
dc.contributor.other Chemical Engineering
dc.date.accessioned 2024-07-05T14:25:56Z
dc.date.available 2024-07-05T14:25:56Z
dc.date.issued 2014
dc.department Atılım University en_US
dc.department-temp [Durak, Halil; Gulcan, Mehmet; Zahmakiran, Mehmet] Yuzuncu Yil Univ, Fac Sci, Dept Chem, TR-65080 Van, Turkey; [Ozkar, Saim] Middle E Tech Univ, Dept Chem, TR-06800 Ankara, Turkey; [Kaya, Murat] Atilim Univ, Dept Chem Engn & Appl Chem, TR-06836 Ankara, Turkey en_US
dc.description Ozkar, S/0000-0002-6302-1429; Kaya, Murat/0000-0002-2458-8924; Gulcan, Mehmet/0000-0002-3921-8811 en_US
dc.description.abstract The development of readily prepared effective heterogeneous catalysts for hydrogen generation from ammonia-borane (AB; NH3BH3) solution under mild conditions still remains a challenge in the field of "hydrogen economy". In this study, we report our finding of an in situ generated, highly active ruthenium nanocatalyst for the dehydrogenation of ammonia-borane in water at room temperature. The new catalyst system consists of ruthenium(0) nanoparticles supported on nanohydroxyapatite (RuNPs@nano-HAp), and can be reproducibly prepared under in situ conditions from the ammonia-borane reduction of Ru3+ ions exchanged into nanohydroxyapatite (Ru3+@nano-HAp) during the hydrolytic dehydrogenation of ammonia-borane at 25 +/- 0.1 degrees C. Nanohydroxyapatite-supported ruthenium(0) nanoparticles were characterized by a combination of advanced analytical techniques. The sum of their results shows the formation of well-dispersed ruthenium(0) nanoparticles with a mean diameter of 2.6 +/- 0.6 nm on the surface of the nanospheres of hydroxyapatite by keeping the host matrix intact. The resulting RuNPs@nano-HAp are highly active catalyst in the hydrolytic dehydrogenation of ammonia-borane with an initial TOF value of 205 min(-1) by generating 3.0 equiv. of H-2 per mole of ammonia-borane at 25 +/- 0.1 degrees C. Moreover, they are sufficiently stable to be isolated and bottled as solid materials, which can be reused as active catalyst under the identical conditions of first run. The work reported here also includes the following results: (i) monitoring the formation kinetics of the in situ generated RuNPs@nano-HAp by hydrogen generation from the hydrolytic dehydrogenation of ammonia-borane as the reporter reaction. The sigmoidal kinetics of catalyst formation and concomitant dehydrogenation fits well to the two-step, slow nucleation, followed by autocatalytic surface growth mechanism, P -> Q (rate constant k(1)) and P + Q -> 2Q (rate constant k(2)), in which P is Ru3+@nano-HAp and Q is the growing, catalytically active RuNPs@nano-HAp; (ii) the compilation of kinetic data for the RuNPs@nano-HAp catalyzed hydrolytic dehydrogenation of ammonia-borane depending on the temperature and catalyst concentration to determine the dependency of reaction rate on catalyst concentration and activation parameters (E-a, Delta H-#, and Delta S-#) of the reaction. en_US
dc.description.sponsorship Turkish Academy of Sciences; FABED en_US
dc.description.sponsorship Partial support by the Turkish Academy of Sciences is gratefully acknowledged. MZ thanks FABED for their partial support to his research. en_US
dc.identifier.citationcount 32
dc.identifier.doi 10.1039/c4ra03213f
dc.identifier.endpage 28955 en_US
dc.identifier.issn 2046-2069
dc.identifier.issue 55 en_US
dc.identifier.scopus 2-s2.0-84904134660
dc.identifier.scopusquality Q1
dc.identifier.startpage 28947 en_US
dc.identifier.uri https://doi.org/10.1039/c4ra03213f
dc.identifier.uri https://hdl.handle.net/20.500.14411/64
dc.identifier.volume 4 en_US
dc.identifier.wos WOS:000339554500022
dc.identifier.wosquality Q2
dc.institutionauthor Kaya, Murat
dc.language.iso en en_US
dc.publisher Royal Soc Chemistry en_US
dc.relation.publicationcategory Makale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı en_US
dc.rights info:eu-repo/semantics/closedAccess en_US
dc.scopus.citedbyCount 37
dc.subject [No Keyword Available] en_US
dc.title Hydroxyapatite-Nanosphere Supported Ruthenium(0) Nanoparticle Catalyst for Hydrogen Generation From Ammonia-Borane Solution: Kinetic Studies for Nanoparticle Formation and Hydrogen Evolution en_US
dc.type Article en_US
dc.wos.citedbyCount 34
dspace.entity.type Publication
relation.isAuthorOfPublication bac01133-1748-4faf-996a-38f013299b7d
relation.isAuthorOfPublication.latestForDiscovery bac01133-1748-4faf-996a-38f013299b7d
relation.isOrgUnitOfPublication bebae599-17cc-4f0b-997b-a4164a19b94b
relation.isOrgUnitOfPublication.latestForDiscovery bebae599-17cc-4f0b-997b-a4164a19b94b

Files

Collections