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    Group 4 oxides supported Rhodium(0) catalysts in hydrolytic dehydrogenation of ammonia borane
    (Pergamon-Elsevier Science Ltd, 2019) Tonbul, Yalcin; Akbayrak, Serdar; Ozkar, Saim
    Rh3+ ions are first impregnated on Group 4 metal oxides (TiO2, ZrO2, HfO2) in aqueous solution and, then reduced with aqueous solution of NaBH4 to form rhodium(0) nanoparticles (NPs) on the oxide surface. The analyses reveal that Rh(0) NPs are highly dispersed on the surface of TiO2, ZrO2, HfO2. Rh-0/MO2 (M: Ti, Zr, Hf) NPs have high activity and reusability in releasing H-2 from the hydrolysis of ammonia borane with an initial turnover frequency of 643, 198, and 188 min(-1), respectively, at 25.0 +/- 0.1 degrees C. The reusability of Rh-0/ZrO2 and Rh-0/HfO2 catalysts is higher than that of the Rh-0/TiO2 catalyst. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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    Magnetically Separable Rh0/Co3O4 Nanocatalyst Provides over a Million Turnovers in Hydrogen Release from Ammonia Borane
    (Amer Chemical Soc, 2020) Akbayrak, Serdar; Tonbul, Yalcin; Ozkar, Saim
    Cobalt(II,III) oxide nanopowders are used as supporting materials for rhodium(0) nanoparticles forming Rh-0/Co3O4 nanocatalysts, which can be prepared by impregnation and sodium borohydride reduction of Rh3+ ions on the surface of the oxide support. Magnetically separable Rh-0/Co3O4 nanoparticles are isolated from the reaction medium by an external magnet and characterized using various analytical techniques. Rh-0/Co3O4 nanoparticles are highly active and reusable catalysts with a long lifetime in hydrolytic dehydrogenation of ammonia borane (AB) at room temperature. Rh-0/Co3O4 nanoparticles with 0.5% wt Rh loading provide a turnover frequency of 1800 min(-1) and a total of 1.02 x 10(6) turnovers for H-2 evolution from the hydrolysis of AB at 25.0 +/- 0.1 degrees C. This turnover frequency is the second best value ever reported for the hydrolysis of AB, and the total turnover number of over a million is a record lifetime ever reported. Magnetically separable rhodium(0) nanoparticles are expectedly highly reusable catalysts and preserve their initial activity after the fifth run of hydrolysis. We also report the results of our study on the catalytic activity of Co3O4 nanopowders for the same dehydrogenation reaction.
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    Magnetically separable rhodium nanoparticles as catalysts for releasing hydrogen from the hydrolysis of ammonia borane
    (Academic Press Inc Elsevier Science, 2019) Tonbul, Yalcin; Akbayrak, Serdar; Ozkar, Saim
    Magnetically separable catalysts attract considerable attention in catalysis due to their facile separation from the reaction medium. This propensity is crucial for efficient multiple use of precious noble metal nanoparticles in catalysis. In fact, the isolation of catalysts from the reaction medium by filtration and washing results usually in the loss of huge amount of activity in the subsequent run of catalysis. Although many transition metal nanoparticle catalysts have been reported for the H-2 generation from the hydrolysis of ammonia borane, there is no study reporting the magnetically separable rhodium based catalysts for the hydrolytic dehydrogenation of ammonia borane. Here, we report the preparation of rhodium(0) nanoparticles supported on the surface of Fe3O4 and CoFe2O4 magnetic nanopowders as the first example of magnetically separable rhodium nanocatalysts. The resulting magnetically separable Rh-0/Fe3O4 and Rh-0/CoFe2O4 nanoparticles are highly active, long-lived and reusable catalysts in H-2 generation from the hydrolysis of ammonia borane providing a turnover frequency value of 273 and 720 min(-1), respectively, at 25.0 +/- 0.1 degrees C. These magnetically separable catalysts show high reusability and long-term stability in the hydrolysis reaction. They retain their complete initial activity even after the 5th use releasing exactly 3.0 equivalent H-2 gas per mole of ammonia borane. The long-term stability tests show that Rh-0/Fe3O4 and Rh-0/CoFe2O4 nanoparticles provide a total turnover number of 125,000 and 245,000, respectively, in releasing H-2 from the hydrolysis of ammonia borane at room temperature. The long term stability and reusability of magnetically separable Rh-0/Fe3O4 and Rh-0/CoFe2O4 nanopartides make them attractive catalysts for hydrogen generation in fuel cell applications. (C) 2019 Elsevier Inc. All rights reserved.
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    Nanozirconia supported ruthenium(0) nanoparticles: Highly active and reusable catalyst in hydrolytic dehydrogenation of ammonia borane
    (Academic Press Inc Elsevier Science, 2018) Tonbul, Yalcin; Akbayrak, Serdar; Ozkar, Saim
    Nanozirconia supported ruthenium(0) nanoparticles (Ru-0/ZrO2) were prepared by impregnation of ruthenium(III) cations on the surface of zirconia followed by their reduction with sodium borohydride at room temperature. Ru-0/ZrO2 was isolated from the reaction solution by centrifugation and characterized by ICP-OES, XRD, TEM, SEM EDS and XPS techniques. All the results reveal that ruthenium(0) nanoparticles were successfully supported on zirconia and the resulting Ru-0/ZrO2 is a highly active and reusable catalyst for hydrogen generation from the hydrolysis of ammonia borane with a turnover frequency value of 173 min(-1) at 25 degrees C. The reusability and catalytic lifetime tests reveal that Ru-0/ZrO2 is still active in the subsequent runs of hydrolysis of ammonia borane preserving 67% of the initial catalytic activity even after the fifth run and Ru-0/ZrO2 provides 72,500 turnovers (mol H-2/mol Ru) before deactivation at 25 degrees C. Our report also includes the results of kinetic studies depending on the catalyst concentration and temperature to determine the activation energy (E-a = 58 2 kJ/mol) for hydrolytic dehydrogenation of AB. (C) 2017 Elsevier Inc. All rights reserved.
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    Tungsten(VI) oxide supported rhodium nanoparticles: Highly active catalysts in hydrogen generation from ammonia borane
    (Pergamon-Elsevier Science Ltd, 2021) Akbayrak, Serdar; Tonbul, Yalcin; Ozkar, Saim
    Herein, we report the use of tungsten(VI) oxide (WO3) as support for Rh0 nanoparticles. The resulting Rh0/WO3 nanoparticles are highly active and stable catalysts in H2 generation from the hydrolysis of ammonia borane (AB). We present the results of our investigation on the particle size distribution, catalytic activity and stability of Rh0/WO3 catalysts with 0.5%, 1.0%, 2.0% wt. Rh loadings in the hydrolysis reaction. The results reveal that Rh-0/WO3 (0.5% wt. Rh) is very promising catalyst providing a turnover frequency of 749 min-1 in releasing 3.0 equivalent H2 per mole of AB from the hydrolysis at 25.0 C-circle. The high catalytic activity of Rh-0/WO3 catalyst is attributed to the reducible nature of support. The report covers the results of kinetics study as well as comparative investigation of activity, recyclability, and reusability of colloidal(0) nanoparticles and Rh-0/WO3 (0.5 % wt. Rh) catalyst in the hydrolysis reaction. (c) 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.