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【Nature文章】Three-dimensional atomic-scale structure of size-selected gold nanoclu

已有 4393 次阅读 2008-1-3 11:48 |个人分类:催化资源收藏



Letter

Nature 451, 46-48 (3 January 2008) | doidoidoi:10.1038/nature06470; Received 22 June 2007; Accepted 13 November 2007; Published online 9 December 2007

Three-dimensional atomic-scale structure of size-selected gold nanoclusters

Z. Y. Li1, N. P. Young1, M. Di Vece1, S. Palomba1, R. E. Palmer1, A. L. Bleloch3, B. C. Curley2, R. L. Johnston2, J. Jiang4 & J. Yuan4

  1. Nanoscale Physics Research Laboratory, School of Physics and Astronomy,
  2. School of Chemistry, University of Birmingham, Birmingham B15 2TT, UK
  3. UK SuperSTEM Laboratory, Daresbury Laboratory, Daresbury WA4 4AD, UK
  4. Beijing Electron Microscopy Centre; Laboratory of Advanced Materials and Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

Correspondence to: Z. Y. Li1 Correspondence and requests for materials should be addressed to Z.Y.L. (Email: ziyouli@nprl.ph.bham.ac.uk).

An unambiguous determination of the three-dimensional structure of nanoparticles is challenging1. Electron tomography requires a series of images taken for many different specimen orientations2. This approach is ideal for stable and stationary structures3. But ultrasmall nanoparticles are intrinsically structurally unstable and may interact with the incident electron beam4, 5, 6, constraining the electron beam density that can be used and the duration of the observation. Here we use aberration-corrected scanning transmission electron microscopy7, coupled with simple imaging simulation, to determine with atomic resolution the size, three-dimensional shape, orientation and atomic arrangement of size-selected gold nanoclusters that are preformed in the gas phase and soft-landed on an amorphous carbon substrate. The structures of gold nanoclusters containing 309plusminus6 atoms can be identified with either Ino-decahedral, cuboctahedral or icosahedral geometries. Comparison with theoretical modelling of the system suggests that the structures are consistent with energetic considerations. The discovery that nanoscale gold particles function as active and selective catalysts for a variety of important chemical reactions has provoked much research interest in recent years8, 9, 10, 11, 12. We believe that the detailed structure information we provide will help to unravel the role of these nanoclusters in size- and structure-specific catalytic reactions11, 12. We note that the technique will be of use in investigations of other supported ultrasmall metal cluster systems.


    

References

   8. Haruta, M. Size- and support-dependency in the catalysis of gold. Catal. Today 36, 153–166 (1997) |
  9. Sanchez, A. et al. When gold is not noble: nanoscale gold catalysts. J. Phys. Chem. A 103, 9573–9578 (1999) |
 10. Hughes, M. D. et al. Tunable gold catalysts for selective hydrocarbon oxidation under mild conditions. Nature 437, 1132–1135 (2005) |
  11. Tsunoyama, H., Sakurai, H., Negishi, Y. & Tsukuda, T. Size-specific catalytic activity of polymer-stabilized gold nanoclusters for aerobic alcohol oxidation in water. J. Am. Chem. Soc. 127, 9374–9375 (2005)
  12. Chen, M. S. & Goodman, D. W. Structure-activity relationships in supported Au catalysts. Catal. Today 111, 22–33 (2006) | 


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