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.
Similar content being viewed by others
References
D. K. Shuh. “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. 125 – 134, Karlsruhe, Germany, September 2006.
H. Bluhm, K. Andersson, T. Araki, K. Benzerara, G. E. Brown, J. J. Dynes, S. Ghosal, M. K. Gilles, H. C. Hansen, J. C. Hemminger, A. P. Hitchcock, G. Ketteler, A. L. D. Kilcoyne, E. Kneedler, J. R. Lawrence, G. G. Leppard, J. Majzlam, B. S. Mun, S. C. B. Myneni, A. Nilsson, H. Ogasawara, D. F. Ogletree, K. Pecher, M. Salmeron, D. K. Shuh, B. Tonner, T. Tyliszczak, T. Warwick, and T. H. Yoon, J. Electron Spectrosc., 150, 86–104 (2006).
H. Nilsson, T. Tyliszczak, R. E. Wilson, L. Werme, and D. K. Shuh, Anal. Bioanal. Chem. 383, 41–47 (2005).
H. Nilsson, T. Tyliszczak, R. E. Wilson, L. Werme, and D. K. Shuh. “Soft x-ray spectromicroscopy of actinide particulates”, in Recent Advances in Actinide Science, eds. I. May, R. Alvares, and N. Bryan, Cambridge (2006).
C. Fillaux, C. Den Auwer, D. Guillaumont, D. K. Shuh, and T. Tyliszczak, J. Alloy. Compd. 444–445, 443–446 (2007).
C. Fillaux, J.-C. Berthet, S. D. Conradson, P. Guilbaud, D. Guillaumont, C. Hennig, P. Moisy, J. Roques, E. Simoni, D. K. Shuh, T. Tyliszczak, I. Castro-Rodriguez, and C. Den Auwer, C. R. Chim. 10, 859–871 (2007).
N. Vigier, C. Den Auwer, C. Fillaux, A. Maslennikov, H. Noel, J. Roques, D. K. Shuh, E. Simoni, T. Tyliszczak, and P. Moisy, Chem. Mater. 20, 3199–3204 (2008).
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).
A. W. Addison and P. J. Burke, J. Heterocyclic Chem. 18, 803–805 (1981).
J. A. Hermann and J. F. Suttle, Inorg. Syn. 5,143–145 (1957).
E. Apen, A. P. Hitchcock, and J. L. Gland, J. Phys. Chem. 97, 6859–6866 (1993).
G. Vall-llosera, B. Gao, A. Kivimaeki, M. Coreno, J. A. Ruiz, M. de Simone, H. Agren, and E. Rachlew, J. Chem. Phys, 128, 044316 (2008).
J. Stöhr, NEXAFS spectroscopy, volume 25. Springer-Verlag, Berlin (1992).
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Janousch, M., Copping, R., Tyliszczak, T. et al. Scanning Transmission X-ray Spectromicroscopy of Actinide Complexes. MRS Online Proceedings Library 1104, 606 (2008). https://doi.org/10.1557/PROC-1104-NN06-06
Received:
Accepted:
Published:
DOI: https://doi.org/10.1557/PROC-1104-NN06-06