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Synchrotron-Based X-Ray Spectromicroscopy of Organic Nanoparticles Complexing Actinides

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Actinide Nanoparticle Research

Abstract

Humic acids (HA) have a high binding capacity toward traces of toxic metal cations, including actinides, and have a propensity for forming nano- to micron-sized colloids. They can therefore act as transport vehicles for actinides in aquatic systems, which can have detrimental consequences for the safety of nuclear waste disposal. Modern scanning transmission X-ray microscopy (STXM) at the carbon K(1s)-edge is an excellent tool for investigations of such and other processes. STXM studies, combined with other sophisticated techniques and quantum chemical calculations, provide the necessary spatial resolution in the sub-μm range to resolve characteristic aggregate morphologies and identify molecular processes involved in HA–actinide interaction. Systematic experimental and theoretical investigations of reference systems allow successful interpretation of C 1s near edge X-ray absorption fine structure (NEXAFS) extracted from STXM image stacks of HA–metal aggregates. The results show that different HA domains (of likely structurally supramolecular HA associations) exhibit different interactions with metal cations. Metal cations bound to HA are enriched in a minority fraction containing higher densities of complexing carboxylic sites. This fraction is likely to play a dominant role in HA colloid-mediated transport of actinides and other toxic trace metals in the hydrosphere.

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Reference

  1. V. Neck, M. Altmaier, T. Fanghaenel, in: R. Alvarez, N.D. Bryan, I May (Eds.), Ad-vances in Actinide Science, Royal Society of Chemistry Publishing, Cambridge 2006, 479–484

    Google Scholar 

  2. http://www.lightsources.org

  3. Ch. David, F. Nolting, Ch. Quitmann, M. Stampanoni, F. Pfeiffer (Eds.), Proceedings of the 9th International Conference on X-Ray Microscopy, Journal of Physics: Conference Series, IOP Publishing, Bristol 2009

    Google Scholar 

  4. P. Horowitz, J.A. Howell, Science 178 (1972) 608–611

    Article  CAS  Google Scholar 

  5. P. Kirkpatrick, A.V. Baez, J. Optical Soc. Am. 38 (1948) 766–774

    CAS  Google Scholar 

  6. Y. Yan, W. M. Gibson, JCPDS-International Centre for Diffraction Data, Adv. X-Ray Anal. 45 (2002) 298–305

    CAS  Google Scholar 

  7. A.G. Michette, Optical Systems for Soft X-Rays, Plenum Press, London 1986

    Google Scholar 

  8. A. Snigirev, V. Kohn, I. Snigireva, B. Lengeler, Nature 384 (1996) 49–51

    Article  CAS  Google Scholar 

  9. http://www.xradia.com/technology/microscopes/types-of-xray-microscopes.php

  10. B. Hornberger, M.D. de Jonge, M. Feser, P. Holl, C. Holzner, C. Jacobsen, D. Legnini, D. Paterson, P. Rehak, L. Strüder, S. Vogt, J. Synchrotron Rad. 15 (2008) 355

    Article  CAS  Google Scholar 

  11. W. Chao, B.D. Harteneck, J. Alexander Liddle, E.H. Anderson, D.T. Attwood, Nature 435 (2005) 1210–1213

    Article  CAS  Google Scholar 

  12. W.H. McMaster, N.K. Del Grande, J.H. Mallett, J.H. Hubbell, Compilation of X-ray cross sections, Lawrence Livermore National Laboratory Report UCRL-50174 (sec-tion I 1970, section II – section IV 1969)

    Google Scholar 

  13. J. Stöhr, NEXAFS Spectroscopy, Springer Series in Surface Sciences 25, Springer-Verlag, Berlin 1992

    Google Scholar 

  14. A.P. Hitchcock, D.C.J. Mancini, J. Electron Spectrosc. Relat. Phenom. 67 (1994) 1–132

    Article  CAS  Google Scholar 

  15. H. Ade, S.G. Urquhart, in: T.K. Sham (Ed.), Chemical applications of synchrotron radiation, World Scientific Publishing, Singapore 2002, 285–355

    Google Scholar 

  16. O. Dhez, H. Ade, S.G.J. Urquhart, J. Electron Spectrosc. Relat. Phenom. 128 (2003) 85

    Article  CAS  Google Scholar 

  17. O. Plashkevych, L. Yang, O. Vahtras, H. Ågren, L.G.M. Petterson, Chem. Phys. 222 (1997) 125

    Article  CAS  Google Scholar 

  18. V. Carravetta, O. Plashkevych, H. Ågren, Chem. Phys. 263 (2001) 231

    Article  CAS  Google Scholar 

  19. I. Bâldea, B. Schimmelpfennig, M. Plaschke, J. Rothe, J. Schirmer, A.B. Trofimov, Th. Fanghänel, J. Electron Spectrosc. Relat. Phenom. 154 (2007) 109

    Article  Google Scholar 

  20. U. Neuhäusler, C. Jacobsen, D. Schulze, D. Stott, S. Abend, J. Synchrotron Rad. 7 (2000) 110–112

    Google Scholar 

  21. J. Kirz, C. Jacobsen, in: Ch. David et al. (Eds.), Proceedings of the 9th International Conference on X-Ray Microscopy, Journal of Physics: Conference Series, IOP Pub-lishing, Bristol 2009, 012001

    Google Scholar 

  22. B. Niemann, D. Rudolph, G. Schmahl, Appl. Opt. 15 (1976) 1883–1884

    Article  CAS  Google Scholar 

  23. H. Rarback, D. Shu, S.C. Feng, H. Ade, C. Jacobsen, J. Kirz, I. McNulty, Y. Vladimirsky, D.P. Kern, T.H.P.Chang, in: Sayre et al. (Eds.), X-ray Microscopy II, Springer Series in Optical Sciences 67, Springer-Verlag, Berlin 1988

    Google Scholar 

  24. http://xray1.physics.sunysb.edu

  25. http://www.als.lbl.gov/als/microscopes/

  26. http://sls.web.psi.ch/view.php/beamlines/pollux/index.html

  27. http://www.lightsource.ca/experimental/sm.php

  28. http://www.bessy.de/cms.php?idcat=166&changelang=5

  29. http://www.elettra.trieste.it/beamlines/TWINMIC/

  30. http://www.bruker-est.com/synchrotron-inst.html

  31. G.J. Flynn, S. Wirick, L.P. Keller, C. Jacobsen, in: Ch. David et al. (Eds.), Proceed-ings of the 9th International Conference on X-Ray Microscopy, Journal of Physics: Conference Series, IOP Publishing, Bristol 2009, 012085

    Google Scholar 

  32. S.G. Urquhart, A.P. Hitchcock, A.P. Smith, H.W. Ade, W. Lidy, E.G. Rightor, G.E. Mitchell, J. Electron Spectrosc. Relat. Phenom. 100 (1999) 119–135

    Article  CAS  Google Scholar 

  33. S.G. Urquhart, A.P. Smith, H.W. Ade, A.P. Hitchcock, E.G. Rightor, W. Lidy, J. Phys. Chem. B 103 (1999) 4603–4610

    Article  CAS  Google Scholar 

  34. A.P. Hitchcock, I. Koprinarov, T. Tyliszczak, E.G. Rightor, G.E. Mitchell, M.T. Dineen, F. Hayes, W. Lidy, R.D. Priester, S.G. Urquhart, A.P. Smith, H. Ade, Ultramicroscopy 88 (2001) 33–49

    Article  CAS  Google Scholar 

  35. H. Ade, B. Hsiao, Science 262 (1993) 1427–1429

    Article  CAS  Google Scholar 

  36. B. Watts, W.J. Belcher, L. Thomsen, H. Ade, P.C. Dastoor, Macromolecules 42(21) (2009) 8392–8397

    Article  CAS  Google Scholar 

  37. J.J.M. Halls, C.A.Walsh, N.C. Greenham, E.A. Marseglia, R.H. Friend, S.C. Moratti, A.B. Holmes, Nature 376 (1995) 498–500

    Article  CAS  Google Scholar 

  38. B.A. Wilson, V.H. Smith, F. Denoyelles Jr., C.K. Larive, Environ. Sci. Technol. 37 (2003) 1713–19

    Article  CAS  Google Scholar 

  39. J.J. Dynes, J.R. Lawrence, D.R. Korber, G.D.W. Swerhone, G.G. Leppard, A.P. Hitchcock, Sci. Total Environ. 369 (2006) 369–383

    Article  CAS  Google Scholar 

  40. N.S Ranganathan, in: J.M Ascenzi (Ed.), Handbook of disinfection and antiseptics, Marcel Dekker Inc., New York 1996, 235–264

    Google Scholar 

  41. T.H. Yoon, Appl. Spectrosc. Rev. 44 (2009) 91–122

    Article  CAS  Google Scholar 

  42. J. Thieme, J. Sedlmair, S.-C. Gleber, J. Prietzel, J. Coates, K. Eusterhues, G. Abbt-Braun, M. Salome, J. Synchrotron Rad. 17 (2010) 149–157

    CAS  Google Scholar 

  43. J. Thieme, I. McNulty, S. Vogt, D. Paterson, Environ. Sci. Technol. 41 (2007) 6885–6889

    Article  CAS  Google Scholar 

  44. M.A. Denecke, C.M. Marquardt, J. Rothe, K. Dardenne, M.P. Jensen, J. Nucl. Sci. Technol. 3 (2002) 410–413

    Google Scholar 

  45. M.A. Denecke, D. Bublitz, J.I. Kim, H. Moll, I. Farkes, J. Synchrotron Rad. 6 (1999) 394–96

    CAS  Google Scholar 

  46. M.A. Denecke, T. Reich, S. Pompe, M. Bubner, K. H. Heise, H. Nitsche, P. G. Allen, J. J. Bucher, N. M. Edelstein, D. K. Shuh, K. R. Czerwinski, Radiochim. Acta 82 (1998) 103–108

    CAS  Google Scholar 

  47. M.K. Armbruster, B. Schimmelpfennig, M. Plaschke, J. Rothe, M.A. Denecke, R. Klenze, J. Electron Spectrosc. Relat. Phenom. 169 (2009) 51–56

    Article  CAS  Google Scholar 

  48. J. Rothe, M. Plaschke, B. Schimmelpfennig, M.A. Denecke, in: Speciation Techniques and Facilities for Radioactive Materials and Synchrotron Light Sources, Nuclear Energy Agency (NEA), OECD-NEA, Issy-les-Moulineaux, France, No. 6288 (2007) 283

    Google Scholar 

  49. J. Rothe, M. Plaschke, M.A. Denecke, in: B. Hedmann and P. Pianeta (Eds.), X-ray Absorption Fine Structure – XAFS13, American Institute of Physics, CP882, Melville, New York 2007, 193

    Google Scholar 

  50. C. Walther, J. Rothe, M. Fuss, S. Büchner, S. Koltsov, T. Bergmann, Anal. Bioanal. Chem. 388 (2007) 409

    Article  CAS  Google Scholar 

  51. H.-R. Cho, C. Walther, J. Rothe, V. Neck, M.A. Denecke, K. Dardenne, Th. Fanghänel, Anal. Bioanal. Chem. 383 (2005) 28–40

    Article  CAS  Google Scholar 

  52. S.C.B. Myneni, Rev. Min. Geochem. 49 (2002) 485

    Article  CAS  Google Scholar 

  53. J. Thieme, C. Schmidt, G. Abbt-Braun, C. Specht, F.H. Frimmel, in: F.H. Frimmel, G. Abbt-Braun (Eds.), Refractory Organic Substances in the Environment, Wiley, New York 2000

    Google Scholar 

  54. A.C. Scheinost, R. Kretzschmar, I. Christl, C. Jacobsen, Spec. Publ. Roy. Soc. Chem. 273 (2002) 39

    Google Scholar 

  55. M. Plaschke, J. Rothe, T. Schäfer, M.A. Denecke, K. Dardenne, S. Pompe, K.-H. Heise, Coll. Surf. A 197 (2002) 245

    Article  CAS  Google Scholar 

  56. J.I. Kim, G. Buckau, G.H. Li, H. Duschner, N. Psarros, Fresenius J. Anal. Chem. 338 (1990) 245

    Article  CAS  Google Scholar 

  57. M. Plaschke, J. Rothe, M. Altmaier, M.A. Denecke, T. Fanghänel, J. Electron Spectrosc. Relat. Phenom. 148 (2005) 151–57

    Article  CAS  Google Scholar 

  58. J. Rothe, M. Plaschke, M.A. Denecke, Radiochim. Acta 92 (2004) 711

    Article  CAS  Google Scholar 

  59. A. Naber, M. Plaschke, J. Rothe, H. Hofmann, T. Fanghänel, J. Electron Spectrosc. Relat. Phenom. 153 (2006) 71–74

    Article  CAS  Google Scholar 

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Authors and Affiliations

  1. Karlsruhe Institute of Technology (KIT), Institute for Nuclear Waste Disposal, 3640, 76021, Karlsruhe, Germany

    Markus Plaschke, Jörg Rothe & Melissa A. Denecke

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  1. Markus Plaschke
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  2. Jörg Rothe
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  3. Melissa A. Denecke
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Correspondence to Melissa A. Denecke .

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Editors and Affiliations

  1. Dept. Chemistry, Lomonosov Moscow State University, Leninskie Gory 1/3, Moskva, 119992, Russian Federation

    Stepan N. Kalmykov

  2. Inst. Nukleare Entsorgungstechnik, Forschungszentrum Karlsruhe, Karlsruhe, Germany

    Melissa A. Denecke

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Plaschke, M., Rothe, J., Denecke, M.A. (2011). Synchrotron-Based X-Ray Spectromicroscopy of Organic Nanoparticles Complexing Actinides. In: Kalmykov, S., Denecke, M. (eds) Actinide Nanoparticle Research. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-11432-8_6

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