Journal Home > Volume 4 , Issue 12

Magnetically recyclable Au/Co/Fe core–shell nanoparticles (NPs) have been successfully synthesized via a one-step in situ procedure. Transmission electron microscope (TEM), energy dispersive X-ray spectroscopic (EDS), and electron energy-loss spectroscopic (EELS) measurements revealed that the trimetallic Au/Co/Fe NPs have a triple-layered core–shell structure composed of a Au core, a Co-rich inter-layer, and a Fe-rich shell. The Au/Co/Fe core–shell NPs exhibit much higher catalytic activities for hydrolytic dehydrogenation of ammonia borane (NH3BH3, AB) than the monometallic (Au, Co, Fe) or bimetallic (AuCo, AuFe, CoFe) counterparts.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

One-Step Synthesis of Magnetically Recyclable Au/Co/Fe TripleLayered Core–Shell Nanoparticles as Highly Efficient Catalysts for the Hydrolytic Dehydrogenation of Ammonia Borane

Show Author's information Kengo Aranishi1,2Hai-Long Jiang1Tomoki Akita1,4Masatake Haruta3,4Qiang Xu1,2,4( )
National Institute of Advanced Industrial Science and Technology (AIST)IkedaOsaka563-8577Japan
Graduate School of EngineeringKobe UniversityNada KuKobeHyogo657-8501Japan
Graduate School of Urban Environmental SciencesTokyo Metropolitan UniversityMinami-OsawaHachiojiTokyo192-0397Japan
Core Research for Evolutional Science and Technology (CREST)Japan Science and Technology Agency (JST)KawaguchiSaitama332-0012Japan

Abstract

Magnetically recyclable Au/Co/Fe core–shell nanoparticles (NPs) have been successfully synthesized via a one-step in situ procedure. Transmission electron microscope (TEM), energy dispersive X-ray spectroscopic (EDS), and electron energy-loss spectroscopic (EELS) measurements revealed that the trimetallic Au/Co/Fe NPs have a triple-layered core–shell structure composed of a Au core, a Co-rich inter-layer, and a Fe-rich shell. The Au/Co/Fe core–shell NPs exhibit much higher catalytic activities for hydrolytic dehydrogenation of ammonia borane (NH3BH3, AB) than the monometallic (Au, Co, Fe) or bimetallic (AuCo, AuFe, CoFe) counterparts.

Keywords: ammonia borane, heterogeneous catalysis, hydrogen generation, core-shell nanoparticles, Triple-layered

References(42)

1

Toshima, N.; Harada, M.; Yonezawa, T.; Kushihashi, K.; Asakura, K. Structural analysis of polymer-protected Pd/Pt bimetallic clusters as dispersed catalysts by using extended X-ray absorption fine structure spectroscopy. J. Phys. Chem. 1991, 95, 7448–7453.

2

Sun, Y. G.; Xia, Y. N. Shape-controlled synthesis of gold and silver nanoparticles. Science2002, 298, 2176–2179.

3

Toshima, N.; Kanemaru, M.; Shiraishi, Y.; Koga, Y. Spontaneous formation of core/shell bimetallic nanoparticles: A calorimetric study. J. Phys. Chem. B2005, 109, 16326–16331.

4

Wilson, O. M.; Scott, R. W. J.; Garcia-Martinez, J. C.; Crooks, R. M. Synthesis, characterization, and structure-selective extraction of 1-3-nm diameter AuAg dendrimer-encapsulated bimetallic nanoparticles. J. Am. Chem. Soc. 2005, 127, 1015–1024.

5

Tao, F.; Grass, M. E.; Zhang, Y. W.; Butcher, D. R.; Renzas, J. R.; Liu, Z.; Chung, J. Y.; Mun, B. S.; Salmeron, M.; Somorjai, G. A. Reaction-driven restructuring of Rh-Pd and Pt-Pd core-shell nanoparticles. Science 2008, 322, 932–934.

6

Alayoglu, S.; Nilekar, A. U.; Mavrikakis, M.; Eichhorn, B. Ru-Pt core-shell nanoparticles for preferential oxidation of carbon monoxide in hydrogen. Nat. Mater. 2008, 7, 333–338.

7

Yang, J.; Sargent, E. H.; Kelley, S. O.; Ying, J. Y. A general phase-transfer protocol for metal ions and its application in nanocrystal synthesis. Nat. Mater. 2009, 8, 683–689.

8

Lee, Y. W.; Kim, M.; Kim, Z. H.; Han, S. W. One-step synthesis of Au@Pd core-shell nanooctahedron. J. Am. Chem. Soc. 2009, 131, 17036–17037.

9

Kobayashi, H.; Yamauchi, M.; Kitagawa, H.; Kubota, Y.; Kato, K.; Takata, M. Atomic-level Pd-Pt alloying and largely enhanced hydrogen-storage capacity in bimetallic nanoparticles reconstructed from core/shell structure by a process of hydrogen absorption/desorption. J. Am. Chem. Soc. 2010, 132, 5576–5577.

10

Ferrando, R.; Jellinek, J.; Johnston, R. L. Nanoalloys: From theory to applications of alloy clusters and nanoparticles. Chem. Rev. 2008, 108, 845–910.

11

Zhang, Z. Y.; Nenoff, T. M.; Leung, K.; Ferreira, S. R.; Huang, J. Y.; Berry, D. T.; Provencio, P. P.; Stumpft, R. Room-temperature synthesis of Ag-Ni and Pd-Ni alloy nanoparticles. J. Phys. Chem. C2010, 114, 14309–14318.

12

Jiang, H. L.; Umegaki, T.; Akita, T.; Zhang, X. B.; Haruta, M.; Xu, Q. Bimetallic Au-Ni nanoparticles embedded in SiO2 nanospheres: Synergetic catalysis in hydrolytic dehydrogenation of ammonia borane. Chem. Eur. J. 2010, 16, 3132–3137.

13

Wang, D. S.; Li, Y. D. One-pot protocol for Au-based hybrid magnetic nanostructures via a noble-metal-induced reduction process. J. Am. Chem. Soc. 2010, 132, 6280–6281.

14

Jiang, H. L.; Akita, T.; Ishida, T.; Haruta, M.; Xu, Q. Synergistic catalysis of Au@Ag core-shell nanoparticles stabilized on metal-organic framework. J. Am. Chem. Soc. 2011, 133, 1304–1306.

15

Yan, J. M.; Zhang, X. B.; Han, S.; Shioyama, H.; Xu, Q. Magnetically recyclable Fe-Ni alloy catalyzed dehydrogenation of ammonia borane in aqueous solution under ambient atmosphere. J. Power Sources2009, 194, 478–481.

16

Yan, J. M.; Zhang, X. B.; Akita, T.; Haruta, M.; Xu, Q. One-step seeding growth of magnetically recyclable Au@Co core-shell nanoparticles: Highly efficient catalyst for hydrolytic dehydrogenation of ammonia borane. J. Am. Chem. Soc. 2010, 132, 5326–5327.

17

Mazumder, V.; Chi, M. F.; More, K. L.; Sun, S. H. Core/shell Pd/FePt nanoparticles as an active and durable catalyst for the oxygen reduction reaction. J. Am. Chem. Soc. 2010, 132, 7848–7849.

18

Toshima, N.; Ito, R.; Matsushita, T.; Shiraishi, Y. Trimetallic nanoparticles having a Au-core structure. Catal. Today2007, 122, 239–244.

19

Mazumder, V.; Chi, M. F.; More, K. L.; Sun, S. H. Synthesis and characterization of multimetallic Pd/Au and Pd/Au/FePt core/shell nanoparticles. Angew. Chem. Int. Ed. 2010, 49, 9368–9372.

20

Wang, L.; Yamauchi, Y. Autoprogrammed synthesis of triple-layered Au@Pd@Pt core-shell nanoparticles consisting of a Au@Pd bimetallic core and nanoporous Pt Shell. J. Am. Chem. Soc. 2010, 132, 13636–13638.

21

Kitchin, J. R.; Nørskov, J. K.; Barteau, M. A.; Chen, J. G. Role of strain and ligand effects in the modification of the electronic and chemical properties of bimetallic surfaces. Phys. Rev. Lett. 2004, 93, 156801.

22

Hamilton, C. W.; Baker, R. T.; Staubitz, A.; Manners, I. B-N compounds for chemical hydrogen storage. Chem. Soc. Rev. 2009, 38, 279–293.

23

Gutowska, A.; Li, L. Y.; Shin, Y. S.; Wang, C. M. M.; Li, X. H. S.; Linehan, J. C.; Smith, R. S.; Kay, B. D.; Schmid, B.; Shaw, W.; Gutowski, M.; Autrey, T. Nanoscaffold mediates hydrogen release and the reactivity of ammonia borane. Angew. Chem. Int. Ed. 2005, 44, 3578–3582.

24

Bluhm, M. E.; Bradley, M. G.; Butterick, R.; Kusari, U.; Sneddon, L. G. Amineborane-based chemical hydrogen storage: Enhanced ammonia borane dehydrogenation in ionic liquids. J. Am. Chem. Soc. 2006, 128, 7748–7749.

25

Diyabalanage, H. V. K.; Shrestha, R. P.; Semelsberger, T. A.; Scott, B. L.; Bowden, M. E.; Davis, B. L.; Burrell, A. K. Calcium amidotrihydroborate: A hydrogen storage material. Angew. Chem. Int. Ed. 2007, 46, 8995–8997.

26

Xiong, Z. T.; Yong, C. K.; Wu, G. T.; Chen, P.; Shaw, W.; Karkamkar, A.; Autrey, T.; Jones, M. O.; Johnson, S. R.; Edwards, P. P.; David, W. I. F. High-capacity hydrogen storage in lithium and sodium amidoboranes. Nat. Mater. 2008, 7, 138–141.

27

Chandra, M.; Xu, Q. A high-performance hydrogen generation system: Transition metal-catalyzed dissociation and hydrolysis of ammonia-borane. J. Power Sources2006, 156, 190–194.

28

Xu, Q.; Chandra, M. Catalytic activities of non-noble metals for hydrogen generation from aqueous ammonia-borane at room temperature. J. Power Sources2006, 163, 364–370.

29

Xu, Q.; Chandra, M. A portable hydrogen generation system: Catalytic hydrolysis of ammonia-borane. J. Alloys. Compd. 2007, 446, 729–732.

30

Yan, J. M.; Zhang, X. B.; Han, S.; Shioyama, H.; Xu, Q. Iron-nanoparticle-catalyzed hydrolytic dehydrogenation of ammonia borane for chemical hydrogen storage. Angew. Chem. Int. Ed. 2008, 47, 2287–2289.

31

Umegaki, T.; Yan, J. M.; Zhang, X. B.; Shioyama, H.; Kuriyama, N.; Xu, Q. Boron- and nitrogen-based chemical hydrogen storage materials. Int. J. Hydrogen Energy2009, 34, 2303–2311.

32

Jiang, H. L.; Singh, S. K.; Yan, J. M.; Zhang, X. B.; Xu, Q. Liquid-phase chemical hydrogen storage: Catalytic hydrogen generation under ambient conditions. ChemSusChem2010, 3, 541–549.

33

Metin, Ö.; Mazumder, V.; Özkar, S.; Sun, S. S. Monodisperse nickel nanoparticles and their catalysis in hydrolytic dehydrogenation of ammonia borane. J. Am. Chem. Soc. 2010, 132, 1468–1469.

34

Çalışkan, S.; Zahmakiran, M.; Özkar, S. Zeolite confined rhodium(0) nanoclusters as highly active, reusable, and long-lived catalyst in the methanolysis of ammonia-borane. Appl. Catal. B-Environ. 2010, 93, 387–394.

35

Demirci, U. B.; Miele, P. Hydrolysis of solid ammonia borane. J. Power Sources2010, 195, 4030–4035.

36

Jiang, H. L.; Xu, Q. Catalytic hydrolysis of ammonia borane for chemical hydrogen storage. Catal. Today2011, 170, 56–63.

37

Denney, M. C.; Pons, V.; Hebden, T. J.; Heinekey, D. M.; Goldberg, K. I. Efficient catalysis of ammonia borane dehydrogenation. J. Am. Chem. Soc. 2006, 128, 12048–12049.

38

Keaton, R. J.; Blacquiere, J. M.; Baker, R. T. Base metal catalyzed dehydrogenation of ammonia-borane for chemical hydrogen storage. J. Am. Chem. Soc. 2007, 129, 1844–1845.

39

Stephens, F. H.; Pons, V.; Baker, R. T. Ammonia-borane: The hydrogen source par excellence? Dalton Trans. 2007, 2613–2626.

40

Yao, C. F.; Zhuang, L.; Cao, Y. L.; Ai, X. P.; Yang, H. X. Hydrogen release from hydrolysis of borazane on Pt- and Ni-based alloy catalysts. Int. J. Hydrogen Energy2008, 33, 2462–2467.

41

Kalidindi, S. B.; Sanyal, U.; Jagirdar, B. R. Nanostructured Cu and Cu@Cu2O core shell catalysts for hydrogen generation from ammonia-borane. Phys. Chem. Chem. Phys. 2008, 10, 5870–5874.

42

Umegaki, T.; Yan, J. M.; Zhang, X. B.; Shioyama, H.; Kuriyama, N.; Xu, Q. Hollow Ni-SiO2 nanosphere-catalyzed hydrolytic dehydrogenation of ammonia borane for chemical hydrogen storage. J. Power Sources2009, 191, 209–216.

File
12274_2011_174_MOESM1_ESM.pdf (920.6 KB)
Publication history
Copyright
Acknowledgements

Publication history

Received: 23 March 2011
Revised: 13 August 2011
Accepted: 01 September 2011
Published: 10 October 2011
Issue date: December 2011

Copyright

© Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2011

Acknowledgements

Acknowledgements

We thank National Institute of Advanced Industrial Science and Technology (AIST), Kobe University and Japan Science and Technology Agency (JST) for financial support.

Return