Ceria supported rhodium nanoparticles: Superb catalytic activity in hydrogen generation from the hydrolysis of ammonia borane

Date

2016-12-05

Author

Akbayrak, Serdar
Tonbul, Yalcin
Özkar, Saim

Metadata

Show full item record

This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

Item Usage Stats

258
views

0
downloads

We investigated the effect of various oxide supports on the catalytic activity of rhodium nanoparticles in hydrogen generation from the hydrolysis of ammonia borane. Among the oxide supports (CeO2, SiO2, Al2O3, TiO2, ZrO2, HfO2) ceria provides the highest catalytic activity for the rhodium(0) nanoparticles in the hydrolysis of ammonia borane. Rhodium(0) nanoparticles supported on nanoceria (Rh-0/CeO2) were prepared by the impregnation of rhodium(III) ions on the surface of ceria followed by their reduction with sodium borohydride in aqueous solution at room temperature. They were isolated from the reaction solution by centrifugation and characterized by a combination of advanced analytical techniques. The catalytic activity of Rh-0/CeO2 samples with various rhodium loading in the range of 0.1-4.0% wt. Rh was also tested in hydrogen generation from the hydrolysis of ammonia borane at room temperature. The highest catalytic activity was achieved by using 0.1% wt. rhodium loaded nanoceria. The resulting Rh-0/CeO2 with a metal loading of 0.1% wt. Rh show superb catalytic activity in hydrogen generation from the hydrolysis of ammonia borane with a record turnover frequency value (TOF) of 2010 min(-1) at 25.0 +/- 0.1 degrees C. The superb catalytic activity of Rh-0/CeO2 is ascribed to the reducible nature of ceria. The reduction of cerium(IV) to cerium(III) leads to a build-up of negative charge on the oxide surface which favors the bonding of rhodium(0) nanoparticles on the surface and, thus, their catalytic activity. Rh-0/CeO2 are also reusable catalysts preserving 67% of their initial catalytic activity even after the fifth use in hydrogen generation from the hydrolysis of ammonia borane at room temperature (TOF= 1350 min(-1). The work reported here also includes the kinetic studies depending on the temperature to determine the activation energy (E-a = 43 +/- 2 kJ/mol) and the effect of catalyst concentration on the rate of hydrolysis of ammonia borane.

Subject Keywords

Catalytic hydrolysis, Hydrogen generation, Ammonia borane, Rhodium nanoparticles, Ceria

URI

https://hdl.handle.net/11511/42172

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL

DOI

https://doi.org/10.1016/j.apcatb.2016.05.061

Collections

Department of Chemistry, Article

Suggestions

OpenMETU
Core

Ceria supported manganese(0) nanoparticle catalysts for hydrogen generation from the hydrolysis of sodium borohydride DUMAN, SİBEL; Özkar, Saim (2018-08-09) Herein we report for the first time the preparation and catalytic use of the ceria supported manganese(0) nanoparticles in hydrogen generation from the hydrolysis of sodium borohydride. They are in situ formed from the reduction of manganese(II) ions on the surface of ceria nanopowders during the catalytic hydrolysis of sodium borohydride in aqueous solution at room temperature. Manganese(0) nanoparticles are isolated from the reaction solution by centrifugation and characterized by a combination of analyti...
Nanoalumina-supported rhodium(0) nanoparticles as catalyst in hydrogen generation from the methanolysis of ammonia borane Ozhava, Derya; Özkar, Saim (2017-10-01) Rhodium(0) nanoparticles were in situ formed from the reduction of rhodium(II) octanoate and supported on the surface of nanoalumina yielding Rh(0)/nanoAl(2)O(3) which is highly active catalyst in hydrogen generation from the methanolysis of ammonia borane at room temperature. The kinetics of nanoparticle formation can be followed just by monitoring the volume of hydrogen gas evolved from the methanolysis of ammonia borane. The evaluation of the kinetic data gives valuable insights to the slow, continuous n...
Hydrogen generation from the hydrolysis of hydrazine-borane catalyzed by rhodium(0) nanoparticles supported on hydroxyapatite Celik, Derya; Karahan, Senem; Zahmakiran, Mehmet; Özkar, Saim (2012-03-01) Herein, we report the preparation and characterization of rhodium(0) nanoparticles supported on hydroxyapatite (Ca-10(OH)(2)(PO4)(6), HAP) and their catalytic use in the hydrolysis of hydrazine-borane, which attracts recent attention as promising hydrogen storage materials. Hydroxyapatite supported rhodium(0) nanoparticles were readily prepared by the hydrazine-borane reduction of rhodium(III)-exchanged hydroxyapatite in situ during the hydrolysis of hydrazine-borane at room temperature. Characterization of...
Tungsten(VI) oxide supported rhodium nanoparticles: Highly active catalysts in hydrogen generation from ammonia borane Akbayrak, Serdar; Tonbul, Yalcin; Özkar, Saim (2021-04-01) 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 Rh0/WO3 (0.5% wt. Rh) is very promising catalyst providing a turn...
Magnetically Separable Rh-0/Co3O4 Nanocatalyst Provides over a Million Turnovers in Hydrogen Release from Ammonia Borane Akbayrak, Serdar; Tonbul, Yalcin; Özkar, Saim (2020-03-16) 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 hydrolyti...

Citation Formats

S. Akbayrak, Y. Tonbul, and S. Özkar, “Ceria supported rhodium nanoparticles: Superb catalytic activity in hydrogen generation from the hydrolysis of ammonia borane,” APPLIED CATALYSIS B-ENVIRONMENTAL, pp. 162–170, 2016, Accessed: 00, 2020. [Online]. Available: https://hdl.handle.net/11511/42172.