Ruthenium(0) Nanoparticles Supported on Multiwalled Carbon Nanotube As Highly Active Catalyst for Hydrogen Generation from Ammonia-Borane

被引:186
作者
Akbayrak, Serdar [1 ]
Ozkar, Saim [1 ]
机构
[1] Middle E Tech Univ, Dept Chem, TR-06800 Ankara, Turkey
关键词
ruthenium nanoparticles; carbon nanotube; heterogeneous catalyst; hydrogen generation; ammonia borane; hydrolysis; METAL NANOCLUSTER FORMATION; HYDROLYTIC DEHYDROGENATION; PALLADIUM(0) NANOCLUSTERS; RHODIUM(0) NANOCLUSTERS; STABILIZED RUTHENIUM(0); THERMAL-DECOMPOSITION; REUSABLE CATALYST; STORAGE; NUCLEATION; METHANOLYSIS;
D O I
10.1021/am3019146
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Ruthenium(0) nanoparticles supported on multiwalled carbon nanotubes (Ru(0)@MWCNT) were in situ formed during the hydrolysis of ammonia-borane (AB) and could be isolated from the reaction solution by filtration and characterized by ICP-OES, XRD, TEM, SEM, EDX, and XPS techniques. The results reveal that ruthenium(0) nanoparticles of size in the range 1.4-3.0 nm are well-dispersed on multiwalled carbon nanotubes. They were found to be highly active catalyst in hydrogen generation from the hydrolysis of AB with a turnover frequency value of 329 min(-1). The reusability experiments show that Ru(0)@MWCNTs are isolable and redispersible in aqueous solution; when redispersed they are still active catalyst in the hydrolysis of AB exhibiting a release of 3.0 equivalents of H-2 per mole of NH3BH3 and preserving 41% of the initial catalytic activity even after the fourth run of hydrolysis. The lifetime of Ru(0)@MWCNTs was measured as 26400 turnovers over 29 h in the hydrolysis of AB at 25.0 +/- 0.1 degrees C before deactivation. The work reported here also includes the kinetic studies depending on the temperature to determine the activation energy of the reaction (E-a = 33 +/- 2 kJ/mol) and the effect of catalyst concentration on the rate of the catalytic hydrolysis of AB, respectively.
引用
收藏
页码:6302 / 6310
页数:9
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