Encl. 1 - Legnaro National Laboratories

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European Nuclear Science and Applications Research
Grant Agreement n. 262010
TNA03 - Transnational Access to LNL-LNS
Application Form
For each item you may refer to the Guidelines for Application (Encl. 1).
Project Title
Contaminant Migration in radioactive waste repositories by Ion Beam Techniques (COMIBEAT)
Abstract
The global aim of the project is to determine radionuclide (RN) migration (transport and
retention) parameters within the materials selected as barriers in radioactive waste repositories,
especially in high-level deep geological repositories (DGR). A DGR is a multibarrier system that
includes engineered barriers (metal canisters, compacted bentonite clay and cement materials)
emplaced hundred meters depth in a geological formation (typically consolidated clays or granite
formations). Diffusion coefficients and retention parameters for radionuclides (RN), within these
very different and heterogeneous materials, are the fundamental to evaluate the long-term
safety of a repository.
The project proposes the combination of the RBS (Rutherford Backscattering Spectrometry) and
PIXE (micro-Particle Induced X-Ray Emission) techniques, available at the AN2000 accelerator of
the Laboratori Nazionali di Legnaro (LNL-INFN, Padova - Italy), for evaluating diffusion coefficients
and surface retention parameters, accounting for the materials heterogeneity, what cannot be
studied by conventional methodologies. The combined application of both techniques, initiated in
2000, has been demonstrated to be a powerful tool to determine transport parameters,
especially for high sorbing RN. The present configuration, detectors, resolution and acquisition
system of the AN2000 facilities are especially adequate for our studies on heterogeneous
geological materials.
In this proposal, the comparative study of the migration of RN in granite, under oxic or anoxic
conditions, is proposed. Experiments will be carried out on natural granite rocks from the
underground research laboratories of GTS (Grimsel Test Site, Switzerland) and Aspö (Sweden,
extracted preserving the natural reducing anoxic conditions occurring 500 m depth in granite. The
study is relevant for redox sensitive RN, since retention mechanisms depends on RN speciation
and the same element under different oxidation states can be mobile or immobile. Experiments
will be started with uranium, selenium, and rhenium, redox sensitive RN very relevant in different
repository scenarios.
The proposed experiments aim to reduce the uncertainties on retention data on crystalline rocks,
specially on redox conditions and heterogeneity, and are included in the EC- CROCK (Crystalline
rock retention processes) Collaborative Project CROCK Fission-2010-1.1.2. FP7- 269658. (20112013) in which our group is participating.
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The project was approved on last July within last USP panel, and two measurements days at the
AN2000 facilities were allocated.
We kindly request for financial support within ENSAR call (period 3rd October 2011–29th February
2012).
Accelerator
Superconducting Cyclotron K800 (LNS)
Tandem-ALPI (LNL)
PIAVE-ALPI
(LNL)
Tandem XTU (LNL)
Tandem SMP (LNS)
Facilities of interest
CN
(LNL)
AN200
(LNL)
Nuclear Structure and Dynamics Based Facilities (NSDBF)
Applied and Interdisciplinary Physics Facilities (AIPF)
Setup of interest
Group Leader
Family name
ALONSO
First name
URSULA
Nationality
SPANISH
Home Institution
CIEMAT
Legal Status of Home Institution(1)
RES
Home Institution Country Code (2)
ES
Position Code (3)
EXP
Address
Avda. Complutense 22, Edif 20 - 28040 Madrid SPAIN
Office Phone
+34 913466139
Home Phone
+34 677795140
e-mail
ursula.alonso@ciemat.es
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(1) UNI=University, RES=Public Research Organisation, SME=Small or Medium Enterprise, PRV=Other
and/or profit or non-profit Private Organisation, OTH = Other Organisation
(2) AL=Albania, AT=Austria, BA=Bosnia and Herzegovina, BE=Belgium, BG=Bulgaria, CH=Switzerland,
CY=Cyprus, CZ=Czech Republic, DE=Germany, DK=Denmark, EE=Estonia, ES=Spain, FI=Finland,
FR=France, GB=United Kingdom, GR=Greece, HR=Croatia, HU=Hungary, IE=Ireland, IL=Israel,
IO=International Organization, IS=Iceland, IT=Italy, LI=Liechtenstein, LT=Lithuania, LU=Luxembourg,
LV=Latvia, ME=Montenegro, MK=Fyrom, MT=Malta, NL=Netherlands, NO=Norway, OT=Other,
PL=Poland, PT=Portugal, RO=Romania, RS=Serbia, SE=Sweden, SI=Slovenia, SK=Slovakia, TR=Turkey.
(3) UND = Undergraduate, PGR = Post graduate (student with a first University degree or equivalent),
PDOC = Post-doc researcher, TEC = Technician, EXP = Experienced researcher (professional
researcher).
Access periods requested
New
user*
Name
Institution
No. of
days
No. of Sex
visits
Age
N
Ursula ALONSO
CIEMAT
4
1
F
35
N
Tiziana MISSANA
CIEMAT
4
1
F
45
Y
Ana BENEDICTO
CIEMAT
4
1
F
25
* Answer YES only if the user has never visited the infrastructure before.
 Answer M (Male) or F (Female).
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Additional information for the User Selection Panel
(e.g. Please note that if you have already applied for Transnational Access funds please recall the
results of previous projects).
The present project is the continuation and development of the CIEMAT experiment first entitled
“RBS and µPIXE study of the clay - mediated contaminant transport at the granite / bentonite
interface of a radioactive repository (HLWR)“. The project, started in 2000, proposed the novel
application of the nuclear ion beam techniques RBS (Rutherford Backscattering Spectrometry)
and PIXE (micro-Particle Induced X-Ray Emission) to determine radionuclide transport
parameters within the barriers of a high-level radioactive waste repository. The project was
supported within the 4th, 5th and 6th European Framework Programmes (Contracts: ERBFMGECT980110, HPRI-1999-CT-00083 and FP6, Contract n. 506065 EURONS- EUROpean Nuclear Structure
research).
The frame of our studies is the long-term performance assessment (PA) of a deep geological
repository for high-level radioactive waste (HLWR). To guarantee the safety of the repository,
quantitative data on the main radionuclide (RN) transport mechanisms, as diffusion coefficients
and specific reactive areas within the barriers are needed. Nonetheless, the influence that the
presence of colloidal particles generated in the repository barriers can have on the migration of
RN it is considered a relevant issue.
The experimental quantification of diffusion and retention on heterogeneous geological materials
by conventional techniques is time consuming and rather complex, amongst all for high sorbing
RN and colloids, and almost no experimental data was available. The application of the RBS and
PIXE techniques has been very fruitful for our studies and many interesting novel results were
obtained.
Within these years the obtained results were included in 8 projects financed by the UE (3), the
Spanish Ministry of Education and Science(2) and the Spanish Agency for Radioactive Waste
Management (ENRESA) (3). Moreover, the results were published in 15 publications in prestigious
journals of the Science Citation Index and were part of a PhD Thesis.
Main achievements obtained so far within this project are below summarized.
In the initial stage of the project, the RBS was applied to study the uranium diffusion within
granite (Alonso et al, J. of Contam. Hydrology 61/1-4, 95-10, 2003). Comparable diffusion
coefficients to others reported in the literature were obtained, validating the methodology. It was
possible to demonstrate that bentonite particles could access to the granite, never measured
before (Alonso et al, NIMB 207 /2, 195, 2003). Different retention behavior, in the presence and
in the absence of the clay was observed by qualitative PIXE measurements (Alonso et al, MRS
807, 621-626, 2004) (Missana et al, J. Iberian Geology 32(1) 55-78, 2006). Since the granite pore
structure studies revealed that there were differences depending on the minerals and granite
mineral studied diffusion coefficients were related to the granite heterogeneous pore structure.
It is noteworthy the application to assess the relevance of colloids on the migration of RN within
granite, since no previous experimental data was available. By RBS it was possible to determine,
for the first time, bentonite colloid diffusion coefficient in granite (Alonso et al, Physics and
Chemistry of Earth 32, 469-476, 2007). Further, the colloid diffusion within granite was studied as
function of the colloid diameter. It was possible to determine diffusion coefficients for all
diameters from 2 to 100 nm colloids, while it was demonstrated that the colloid access for the
250 nm colloids was hindered (Alonso et al, Earth & Planetary Sci. Letters 259, 3 2007). For these
colloid-related studies, it was necessary to perform a thorough analysis to validate the
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methodology and to analyse colloid diffusion within a rough surface to differentiate amongst
surface roughness, particle retention and colloid permeation (Patelli et al, NIMB 249, Iss. 1-2,
575-578, 2006).
The colloid surface retention was initially qualitatively analysed (Alonso et al, MRS 807, 621-626,
2004).
In addition, since the RBS technique was especially adequate to determine diffusion coefficients
within low permeability medium for high-sorbing RN, which cannot be generally determined by
conventional techniques, the RN diffusion studies were extended to consolidated clays, another
of the natural media considered as host rocks of the HLWR in clearly shorter times than
conventional approaches (Alonso et al, Appl. Clay Sci. 43 Iss. 3-4, 477-484, 2009). Moreover,
colloid diffusion coefficients were first measured in compacted bentonite and consolidated clay
barriers evaluating compaction density and colloid size effects (Alonso et al, Physics and Chem
Earth, In press).
Many efforts were devoted last years, from LNL participants and from our side, to extend the
initial qualitative PIXE retention results to quantitative studies. Colloid retention distribution
coefficients could be measured on granite at mineral scale, for the first time, accounting for
different geochemical conditions (Alonso et al, Colloids & Surf. A: Physicochem. & Eng. Asp. 347,
230-238, 2009).
This very recent evolution to obtain quantitative radionuclide and colloid distribution coefficients
on selected areas in heterogeneous materials is, at present, specially powerful for our studies and
experiments on cement materials, engineered barriers in temporal and permanent radioactive
waste repositories for low level, intermediate and high level waste repositories were initiated
(Alonso et al, MRS 1124 2009).
The present configuration, detectors, resolution and acquisition system and analytical programs
of the AN2000 facilities are especially adequate for our studies on heterogeneous geological
materials. The collaboration with the AN2000 group has been always very positive and fruitful.
The access to LNL facilities and the EU financial support is fundamental for the progress of our
studies, that will be hopefully extended and developed within the projects in which our Sorption ,
Migration and Colloids Unit of CIEMAT (Spain) is participating and will participate in next future.
Apart from the former experienced group, two PhD students will be involved in the project.
I confirm that the user group has looked over the provisions stated in Annex II (General
Conditions) and Annex III (Specific Provisions for Transnational Access Activities) of the Grant
Agreement ENSAR (n. 262010) and, in particular, the topics III.5 - Confidentiality and III.6 Publicity.
Date
Group Leader signature
…29th September 2011…………………
Ursula Alonso
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…
Encl. 1
Guidelines for Application
Project Title
Indicate the title of the project. Avoid any special character. You are not allowed to use
acronyms that infringe existing trademarks, registered patents and other similar rights.
Abstract
A short description of the project.
Group Researchers
Since these data have to be submitted to EC offices to obtain their approval, the list of
names must be precise. Home Institution should be specified for each researcher only if
different from the Group Leader Home Institution (for other information see the INFNENSAR web page available at the following address http://www.lnl.infn.it/~ENSAR).
Accelerator
Tick the accelerator chosen. Information concerning the available beams can be found in
the LNL/LNS web pages dedicated to the accelerators.
Facility of interest
Tick the facility chosen. Information concerning the facilities can be found in the LNL/LNS
web pages dedicated to the research facilities.
Setup of interest
State the existing experimental setup you intend to use or the name of the setup you
intend to bring and install at LNL/LNS. In the latter case, setup specifications must be
included in the proposal description.
Group Leader
In case of more researchers, the Group Leader is the person in charge of coordinating the
Project Application for all participants. For the Legal Status of Home Institution, Home
Institution Country and Position, use only the code specified in the footnotes (1, 2 and 3).
Please note that the nationality of the Group Leader must be different from the Italian
one.
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Access periods requested
Indicate the names of the users involved in the project, the belonging institution (it should
be specified for each involved researcher only if different from the Group Leader Home
Institution - for other information see the INFN-ENSAR web page available at the following
address http://www.lnl.infn.it/~ENSAR), the number of days that they will spend at
LNL/LNS and the number of visits.
Additional information for the User Selection Panel
Add any additional information you think might helpful to the User Selection Panel for the
evaluation of your proposal (e.g. Where applicable, a brief report on the status of any
experiment performed in previous periods should be also given).
The application form and a copy of the scientific proposal submitted to the Program Advisory
Committees must be sent by e-mail as PDF attachments to lnlensar@lnl.infn.it (PLEASE send
only the first 4 pages concerning the information on the project and the research team involved
– excluding the pages containing the Guidelines).
Alternatively applications may be also faxed to the following address:
Scientific Coordinator of the Transnational Access to LNL-LNS research infrastructures
Dr. Enrico Fioretto
INFN-LNL Laboratori Nazionali di Legnaro
Viale dell'Università, 2
I-35020 Legnaro (Padova)
Tel. +39-049-80.68.437 or 566
Fax. +39-049-80.68.514
e-mail: lnlensar@lnl.infn.it
The Group Leader has also to fill in the worksheet “ListOfUsers.xls” where detailed information
concerning all group members has to be collected as requested by the EC database. Please,
send this file as attachment in the same e-mail.
Any additional request of information can be addressed to: lnlensar@lnl.infn.it
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