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Hollow silica-alumina composite spheres were prepared by a polystyrene (PS) template method using various amounts of PS suspension. Homogeneous hollow spheres prepared using 40 g were found to be with a diameter of about 300 nm in scanning electron microscopy, and transmission electron microscopy demonstrated their hollow sphere morphology. From the nitrogen adsorption isotherm results, the homogeneous hollow spheres prepared using 40 g of the PS suspension were found to be an ordered pore structure. The activities of the hollow spheres prepared using various amounts of the PS suspension for hydrolytic dehydrogenation of ammonia borane were compared. The results showed that 10, 7, and 6 mL of hydrogen were evolved from the aqueous ammonia borane solution in about 40 min in the presence of the hollow spheres prepared using 40, 80, and 120 g of PS suspension, respectively. The homogeneous hollow spheres with an ordered pore structure showed the highest activity among all the hollow spheres. The amount of acid sites and the coordination number of aluminum active species were characterized using neutralization titration and solid-state 27Al magic angle spinning nuclear magnetic resonance spectroscopy. The homogeneous hollow spheres with an ordered pore structure had high amount of acid sites and 4-coordinated aluminum species. The relative proportion of 4-coordinated aluminum species was related to the dispersion of aluminum species. These results indicate that the homogeneous hollow spheres with an ordered pore structure showed the high activity because of high amount of acid sites induced by the highly dispersed aluminum species.


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Influence of morphology of hollow silica-alumina composite spheres on their activity for hydrolytic dehydrogenation of ammonia borane

Show Author's information Naoki TOYAMAaRyota OGAWAaHaruki INOUEaShinobu OHKIbMasataka TANSHObTadashi SHIMIZUbTetsuo UMEGAKIa( )Yoshiyuki KOJIMAa
Department of Materials & Applied Chemistry, College of Science & Engineering, Nihon University, 1-8-14,Kanda-Surugadai, Chiyoda-Ku, Tokyo 101-8308, Japan
National Institute for Materials Science, 3-13, Sakura, Tsukuba, Ibaraki 305-0003, Japan

Abstract

Hollow silica-alumina composite spheres were prepared by a polystyrene (PS) template method using various amounts of PS suspension. Homogeneous hollow spheres prepared using 40 g were found to be with a diameter of about 300 nm in scanning electron microscopy, and transmission electron microscopy demonstrated their hollow sphere morphology. From the nitrogen adsorption isotherm results, the homogeneous hollow spheres prepared using 40 g of the PS suspension were found to be an ordered pore structure. The activities of the hollow spheres prepared using various amounts of the PS suspension for hydrolytic dehydrogenation of ammonia borane were compared. The results showed that 10, 7, and 6 mL of hydrogen were evolved from the aqueous ammonia borane solution in about 40 min in the presence of the hollow spheres prepared using 40, 80, and 120 g of PS suspension, respectively. The homogeneous hollow spheres with an ordered pore structure showed the highest activity among all the hollow spheres. The amount of acid sites and the coordination number of aluminum active species were characterized using neutralization titration and solid-state 27Al magic angle spinning nuclear magnetic resonance spectroscopy. The homogeneous hollow spheres with an ordered pore structure had high amount of acid sites and 4-coordinated aluminum species. The relative proportion of 4-coordinated aluminum species was related to the dispersion of aluminum species. These results indicate that the homogeneous hollow spheres with an ordered pore structure showed the high activity because of high amount of acid sites induced by the highly dispersed aluminum species.

Keywords:

ammonia borane, morphology, hollow silica-alumina composite spheres, dispersion, acid sites
Received: 17 May 2017 Revised: 11 September 2017 Accepted: 21 September 2017 Published: 19 December 2017 Issue date: December 2017
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Publication history

Received: 17 May 2017
Revised: 11 September 2017
Accepted: 21 September 2017
Published: 19 December 2017
Issue date: December 2017

Copyright

© The author(s) 2017

Acknowledgements

This work was supported by NIMS and University of Tokyo microstructural characterization platform as a program of "Nanotechnology Platform" of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. We are grateful to Mr. Deguchi and Ms. Wada for using the solid-state NMR measurement, and Mr. Ito for using the TEM measurement. Additionally, we also thank MicrotracBEL Corp. for using the N2 sorption measurement.

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