Humic Substances in Performance Assessment of Nuclear Waste Disposal

380 Pages·2004·10 MB·English

Forschungszentrum Karlsruhe
in der Helmholtz-Gemeinschaft
Wissenschaftliche Berichte
FZKA 6969

Humic Substances in
Performance Assessment of
Nuclear Waste Disposal:
Actinide and Iodine Migration
in the Far-Field
Second Technical Progress Report

G. Buckau (Editor)
Institut für Nukleare Entsorgung

Juli 2004
Forschungszentrum Karlsruhe
in der Helmholtz-Gemeinschaft

Wissenschaftliche Berichte
FZKA 6969

Humic Substances in Performance Assessment of Nuclear
Waste Disposal: Actinide and Iodine Migration in the Far-Field

Second Technical Progress Report

G. Buckau (Editor)
Institut für Nukleare Entsorgung

Forschungszentrum Karlsruhe GmbH, Karlsruhe
2004
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ISSN 0947-8620

urn:nbn:de:0005-069699
Foreword
The present report describes progress within the second year of the EC-project “Humic
Substances in Performance Assessment of Nuclear Waste Disposal: Actinide and Iodine
Migration in the Far-Field”. Without being a formal requirement of the Commission or co-
funding bodies, this report documents results in great technical detail. It is an open report and
thus makes the detailed results available to a broad scientific community.
The report contains an executive summary written by the coordinator. More detailed results are
given as individual contributions in the form of 23 annexes. Not all results are discussed or
referred to in the executive summary report and thus readers with a deeper interest also need to
consult the annexes.
The report also reflects the successful integration of a temporary contributor via a Marie-Curie
Fellowship (MCFI-2001-01983) (Annex 23). Integration of this activity extends the scope of the
project to a new potential source of humic substances in clay.
Results of the first project year have already been published in a comparable Technical Progress
Report*. For the final year, a comparable report is foreseen.

*: Buckau, G. (Editor) “Humic Substances in Performance Assessment of Nuclear Waste Disposal: Actinide and
Iodine Migration in the Far-Field (First Technical Progress Report)”, Report FZKA 6800, Forschungszentrum
Karlsruhe, Karlsruhe, 2003.
Table of contents

Executive Summary I
Buckau G.

Annex 1 1
Vertical Exchange of Gorleben Fulvic Acids of Different Origin
Schäfer T., Buckau G., Artinger R., Wolf M., Kim J.I., Geyer S., Bleam W.F.,
Wirick S. and Jacobsen C.

Annex 2 13
Migration Case Gorleben
Buckau G., Artinger R. and Kim J.I.

Annex 3 29
Approach for Physico-Chemical Interpretation of An(III) and An(VI) Humate
Complexation.
Buckau G.

Annex 4 45
Comparison of humic colloid mediated transport of plutonium studied by column
experiments with tri- and tetravalent actinide experiments
Artinger R., Kuczewski B., Marquardt C.M., Schäfer T., Seibert A. and Fanghänel Th.

Annex 5 61
NIR Spectroscopic Study on the Influence of Phenolic OH Groups on the
Neptunium(V) Humate Complex Formation
Sachs S. and Bernhard G.

Annex 6 73
Sampling and Characterization of Rock Material from Uranium Mining Waste Rocks
for Study and Modeling of Release and Migration of Uranium
Sachs S., Benes P., Vopalka D., Stamberg K., Mibus J., Bernhard G. and Bauer A.

Annex 7 85
Neptunium(V) Sorption onto Granite and its Mineral Constituents in the Absence and
Presence of Humic Acid
K. Schmeide and G. Bernhard

Annex 8 95
Molecular size and mass distributions of humic substances measured by AFFFF and
TOF-SIMS
Wolf M., Szymczak W., Chanel V. and Buckau G.

Annex 9 111
Isolation and characterization of new batches of Gohy-573
Wolf M., Buckau G. and Geyer S.
Annex 10 125
X-ray Photoelectron Spectroscopy of HUPA organic substances: natural and synthetic
humic compounds
Barré N., Mercier-Bion F. and Reiller P.

Annex 11 139
Prognosticating the humic complexation for redox sensitive actinides through analogy,
using the charge neutralisation model.
Reiller P.

Annex 12 165
Characterisation of fulvic acids by Electrospray with Quadrupole / Time-of-Flight
Mass Spectrometry
Plancque G.

Annex 13 179
Self-Assembled Monolayers of Aminosilanes Chemically Bonded onto Silicon Wafers
for Immobilization of Purified Humic Acids
Barbot C., Pieri J., Durand J.-P., Gourdard F., Plaschke M., Buckau G., Szymczak W.
and Bouloussa O.

Annex 14 213
Determination of Chemical Parameters for the Schlema-Alberoda Uranium Tailings
Pile Migration Case Study.
Bryan N.

Annex 15 225
Mechanistic Modelling of Humic Substance Aggregation Processes
Keepax R.E., Jones D.M. and Bryan N.D.

Annex 16 251
Modelling the Transport of Actinide Elements in the North-Eastern Irish Sea.
Marsden O.J., Abrahamsen L., Gent C., Bryan N.D and Livens F.R.

Annex 17 265
Comparison of Dialysis, Electrophoresis, Ion Exchange and Ultrafiltration as Methods
for Analysis of Complexation of Europium with Humic Acid
Benes P., Stamberg K., Mizera J. and Prochazkova S.

Annex 18 285
Modelling of Kinetics of Complexation and Decomplexation of Eu(III) with Humic
Acid
Stamberg K., Benes P., Mizera J., Vopalka D. and Prochazkova S.

Annex 19 299
Release of americium from humic acid binding sites studied by desorption experimen
using immobilized humic acid silica gel
Szabó G., Guczi J., Miyajima T., Geckeis H. and Bulman R.A.
Annex 20 309
Preliminary results for preparation and characterisation of immobilised humic acid on
silicon wafer
Szabó G., Guczi J., Telegdi J. and Pashalidis I.

Annex 21 319
U(VI) Mono-Hydroxo Humate Complexation
Pashalidis I.

Annex 22 331
Initial studies on temperature impact of humic acid
Pashalidis I., Colocassidou C., Costa C.N., Efstathiou A.M. and Buckau G.

Annex 23 339
Complexation properties of Humic and Fulvic Acids extracted from Callovo-Oxfordian
and Opalinus Clay
Claret F., Schäfer T., Rabung Th., Bauer A., Wolf M. and Buckau G.

EXECUTIVE SUMMARY
HUMIC SUBSTANCES IN PERFORMANCE ASSESSMENT OF
NUCLEAR WASTE DISPOSAL: ACTINIDE AND IODINE MIGRATION
IN THE FAR-FIELD (HUPA)
SECOND TECHNICAL PROGRESS REPORT

EC Contract No.: FIKW-CT-2001-00128
Work period 11.02-10.03)

G. Buckau
(FZK/INE)
I
II