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. 2015 Oct 16:5:15186.
doi: 10.1038/srep15186.

Ruthenium nanoparticles confined in SBA-15 as highly efficient catalyst for hydrolytic dehydrogenation of ammonia borane and hydrazine borane

Qilu Yao  1 , Zhang-Hui Lu  1 , Kangkang Yang  1 , Xiangshu Chen  1 , Meihua Zhu  1
Affiliations

Ruthenium nanoparticles confined in SBA-15 as highly efficient catalyst for hydrolytic dehydrogenation of ammonia borane and hydrazine borane

Qilu Yao et al. Sci Rep. .

Abstract

Ultrafine ruthenium nanoparticles (NPs) within the mesopores of the SBA-15 have been successfully prepared by using a "double solvents" method, in which n-hexane is used as a hydrophobic solvent and RuCl3 aqueous solution is used as a hydrophilic solvent. After the impregnation and reduction processes, the samples were characterized by XRD, TEM, EDX, XPS, N2 adsorption-desorption, and ICP techniques. The TEM images show that small sized Ru NPs with an average size of 3.0 ± 0.8 nm are uniformly dispersed in the mesopores of SBA-15. The as-synthesized Ru@SBA-15 nanocomposites (NCs) display exceptional catalytic activity for hydrogen generation by the hydrolysis of ammonia borane (NH3BH3, AB) and hydrazine borane (N2H4BH3, HB) at room temperature with the turnover frequency (TOF) value of 316 and 706 mol H2 (mol Ru min)(-1), respectively, relatively high values reported so far for the same reaction. The activation energies (Ea) for the hydrolysis of AB and HB catalyzed by Ru@SBA-15 NCs are measured to be 34.8 ± 2 and 41.3 ± 2 kJ mol(-1), respectively. Moreover, Ru@SBA-15 NCs also show satisfied durable stability for the hydrolytic dehydrogenation of AB and HB, respectively.

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Figures

Figure 1
Figure 1
(a) Small-angle and (b) wide-angle XRD patterns for the synthesized Ru@SBA-15 NCs with different Ru loadings.
Figure 2
Figure 2
Nitrogen adsorption-desorption isotherms of the (a) SBA-15, (b) 0.5 wt% Ru@SBA-15, (c) 2.1 wt% Ru@SBA-15, and (d) 4.0 wt% Ru@SBA-15 NCs.
Figure 3
Figure 3
(a–c) TEM images and (d) particle distribution of Ru@SBA-15 NCs with 2.1 wt% Ru loading.
Figure 4
Figure 4. The corresponding EDX spectrum of the Ru@SBA-15 NCs with 2.1 wt% Ru loading.
The Cu signal originates from Cu grid.
Figure 5
Figure 5
X-ray photoelectron (XPS) spectrum of (a) the survey scan and (b) Ru 3d peaks of the Ru@SBA-15 NCs with 2.1 wt% Ru loading.
Figure 6
Figure 6. Hydrogen generation from the hydrolysis of AB (200 mM, 10 mL) catalyzed by Ru@SBA-15 NCs with different Ru loadings at 298 K (Ru/AB = 0.002).
Figure 7
Figure 7
(a) Hydrogen generation from the hydrolysis of AB (200 mM, 10 mL) catalyzed by Ru@SBA-15 NCs at 293–313 K (Ru/AB = 0.002). (b) Arrhenius plot: ln k versus 1/T.
Figure 8
Figure 8
(a) Hydrogen generation from the hydrolysis of HB (200 mM, 10 mL) catalyzed by Ru@SBA-15 NCs at 293–313 K (Ru/HB = 0.002). (b) Arrhenius plot: ln k versus 1/T.
Figure 9
Figure 9
Durability test for the hydrogen generation from aqueous (a) AB and (b) HB solution (200 mM, 10 mL) in the presence of Ru@SBA-15 NCs at 298 K (Ru/AB = 0.002).
See this image and copyright information in PMC

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