Hostname: page-component-cd9895bd7-dk4vv Total loading time: 0 Render date: 2024-12-21T13:20:33.310Z Has data issue: false hasContentIssue false

Scanning Transmission X-ray Spectromicroscopy of Actinide Complexes

Published online by Cambridge University Press:  01 February 2011

David Shuh
Affiliation:
mrjanousch@lbl.gov, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, CA, 94720, United States
Roy Copping
Affiliation:
RCopping@lbl.gov, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, CA, 94720, United States
Tolek Tyliszczak
Affiliation:
Tolek@lbl.gov, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, CA, 94720, United States
Ingrid Castro-Rodriguez
Affiliation:
incasro@gmail.com, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, CA, 94720, United States
David K. Shuh
Affiliation:
dkshuh@lbl.gov, Lawrence Berkeley National Laboratory, Chemical Sciences Division, MS 70A1150, 1 Cyclotron Rd., Berkeley, CA, 94720, United States, 510-486-6937, 510-486-5596
Get access

Abstract

The fundamental characterization and understanding of 5f electron behavior in actinide complexes is imperative to provide an enhanced basis for the rational and accelerated development of improved processes relevant to nuclear energy. Soft x-ray absorption spectroscopy utilizing the scanning transmission x-ray microscope (STXM) at the Advanced Light Source-Molecular Environmental Science (ALS-MES) Beamline 11.0.2 has been used to probe the electronic characteristics of a nitrogen donor ligand 2,6-Bis(2-benzimidazyl)pyridine (BBP) and its resulting U(IV) complex. The nitrogen K- and carbon K-edges have been collected from both ligand and uranium complex, as well as the uranium 4d-edge from the complex. Upon complexation, the light element absorption spectra change markedly and the uranium spectra from the complex is compared to the reference spectrum obtained from U(IV)Cl4. The evolution of the spectral features are described and interpreted within a simple conceptual framework. Based on spectral evidence alone, the uranium is bound through the pyridine-like nitrogens and the oxidation state of the uranium is consistent with a U(IV) species.

Type
Research Article
Copyright
Copyright © Materials Research Society 2008

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

1 Shuh, D. K.. “Scientific Capabilities of the Advanced Light Source for Radioactive Materials”, in Speciation Techniques and Facilities for Radioactive Materials at Synchrotron Light Sources, OECD NEA 6288, pp. 125134, Karlsruhe, Germany, September 2006.Google Scholar
2 Bluhm, H., Andersson, K., Araki, T., Benzerara, K., Brown, G. E. Dynes, J. J. Ghosal, S., Gilles, M. K. Hansen, H. C. Hemminger, J. C. Hitchcock, A. P. Ketteler, G., Kilcoyne, A. L. D. Kneedler, E., Lawrence, J. R. Leppard, G. G. Majzlam, J., Mun, B. S. Myneni, S. C. B. Nilsson, A., Ogasawara, H., Ogletree, D. F. Pecher, K., Salmeron, M., Shuh, D. K. Tonner, B., Tyliszczak, T., Warwick, T., and Yoon, T. H. J. Electron Spectrosc., 150, 86104 (2006).Google Scholar
3 Nilsson, H., Tyliszczak, T., Wilson, R. E. Werme, L., and Shuh, D. K. Anal. Bioanal. Chem. 383, 4147 (2005).Google Scholar
4 Nilsson, H., Tyliszczak, T., Wilson, R. E. Werme, L., and Shuh, D. K.. “Soft x-ray spectromicroscopy of actinide particulates“, in Recent Advances in Actinide Science, eds. May, I. Alvares, R., and Bryan, N., Cambridge (2006).Google Scholar
5 Fillaux, C., Auwer, C. Den, Guillaumont, D., Shuh, D. K. and Tyliszczak, T., J., Alloy. Compd. 444-445, 443446 (2007).Google Scholar
6 Fillaux, C., Berthet, J.-C., Conradson, S. D. Guilbaud, P., Guillaumont, D., Hennig, C., Moisy, P., Roques, J., Simoni, E., Shuh, D. K. Tyliszczak, T., Castro-Rodriguez, I., and Auwer, C. Den, C. R. Chim. 10, 859871 (2007).Google Scholar
7 Vigier, N., Den Auwer, C., Fillaux, C., Maslennikov, A., Noel, H., Roques, J., Shuh, D. K. Simoni, E., Tyliszczak, T., and Moisy, P., Chem. Mater. 20, 31993204 (2008).Google Scholar
8 Report on the Basic Energy Sciences Workshop on Basic Research Needs for Advanced Nuclear Energy Systems, Office of Science, U.S. Department of Energy, Washington, D.C. 20585 (2006).Google Scholar
9 Addison, A. W. and Burke, P. J. J. Heterocyclic Chem. 18, 803805 (1981).Google Scholar
10 Hermann, J. A. and Suttle, J. F. Inorg. Syn. 5,143145 (1957).Google Scholar
11 Apen, E., Hitchcock, A. P. and Gland, J. L. J. Phys. Chem. 97, 68596866 (1993).10.1021/j100128a019Google Scholar
12 Vall-llosera, G., Gao, B., Kivimaeki, A., Coreno, M., Ruiz, J. A. Simone, M. de, Agren, H., and Rachlew, E., J. Chem. Phys, 128, 044316 (2008).Google Scholar
13 Stöhr, J., NEXAFS spectroscopy, volume 25. Springer-Verlag, Berlin (1992).Google Scholar