Fusion Science and Technology

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Leaching Tests of the Tritium Waste Immobilized in

New Cement Mixtures

Viorel Fugaru , Cristian Postolache , Maria Gheorghe , Lidia Radu & Nastasia
Saca

To cite this article: Viorel Fugaru , Cristian Postolache , Maria Gheorghe , Lidia Radu & Nastasia
Saca (2017) Leaching Tests of the Tritium Waste Immobilized in New Cement Mixtures, Fusion
Science and Technology, 71:3, 286-289, DOI: 10.1080/15361055.2017.1293444

To link to this article: https://doi.org/10.1080/15361055.2017.1293444

Published online: 06 Apr 2017.

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 FUSION SCIENCE AND TECHNOLOGY · VOLUME 71 · 286–289 · APRIL 2017
© American Nuclear Society
DOI: http://dx.doi.org/10.1080/15361055.2017.1293444

Leaching Tests of the Tritium Waste Immobilized in New

Cement Mixtures
Viorel Fugaru,a* Cristian Postolache,a Maria Gheorghe,b Lidia Radu,b and Nastasia Sacab
a
Horia Hulubei National Institute of Physics and Nuclear Engineering, 30, Reactorului St, Magurele,
RO 077125, Romania
b
Technical University of Civil Engineering of Bucharest, Lacul Tei Bvd., no. 122–124, RO 020396,
Bucharest, Romania

Received May 15, 2016

Accepted for Publication August 3, 2016

Abstract — The study was conducted in order to determine the immobilization performance of low-
level tritium waste in new cement mixtures. The grouts analyzed are fine mortars, fluid, self- compact-
ing, with flowability, able to fill the smallest gaps in the solid waste container. The grouts curing
showed compact and structural integrity without pores and cracks, so as to ensure radioactive tritium
waste encapsulation.
Two types of solid/liquid tritium radioactive waste with known tritium activity have been prepared: one
type containing a hydrophilic tritium compound and the other one a hydrophobic tritium compound.
The tritium waste was mixed with three different types of grout and poured in a cylindrical mould. The
leaching of tritium from waste solidified/encapsulated in the cement mixtures immersed in an aqueous
environment has been studied in order to select the most appropriate grout type as waste immobilization
matrix.
Samples from the liquid surrounding the cements blocks were collected at predetermined time intervals
and placed in the liquid scintillation cocktail and measured. The activity of the tritium released was then
calculated.

Keywords — Tritium waste, cement, leaching, immobilization.

Note — Some figures may be in color only in the electronic version.

I. INTRODUCTION have some specific properties: a monolithic structure, a low

Immobilization is one of the options for dealing with low
level tritium waste (LLTW), to convert radioactive waste into
a stable form, in order to minimize the release of tradionu-
clides during interim storage, transport and final disposal.
From an economic point of view the waste treatment costs,
as well as the volume and weight of the immobilized waste
form should be as low as possible. Solidification, in terms of
immobilization of the waste, implies both chemical and phy-
sical fixation, with the physical surrounding of the waste with
a barrier (encapsulation). The immobilized LLTW should
*E-mail: vfugaru@nipne.ro
leaching rate, mechanical resistance, resistance to water, resis-
tance to radiolysis and a low overall production cost.1
Cement-based matrix is increasingly being used for
LLTW immobilization and can be considered to be a
suitable option in the confinement of low and intermedi-
ate level waste containing a wide range of radionuclides.2
Although a cement immobilization matrix has a mono-
lithic structure, a gradual release of tritium can be
expected due to the porous structure.
Leaching tests are a means of determining if an
immobilization matrix is acceptable for final disposal in
accordance with the requirements of the regulating
authorities.

286
 LEACHING TESTS OF THE TRITIUM WASTES IN CEMENT MIXTURES · FUGARU et al. 287

The present study has been carried out to evaluate a

new cement mixture, designed for LLTW immobilization,
to reduce tritium release.

II. MATERIALS AND METHODS

II.A. Cementitious Grouts

The cement analyzed – cement-based grouts – are very

fluid fine mortars made out of cement, fillers and fine sand,
namely fine granular material with conventional sand
function. Additionally, high range water reducers (super-
plasticizers admixtures) have been used.
Three types of grout mixes have been prepared and Fig. 1. BR7 grout containers.
were assigned the following codes: BR7, Z5N and G3.
The grouts contain different blended cements:
●
Grout type BR7 paste was poured in special cylindri-
Cement type 1: CEM II/A-V 42.5N with 20%
cally shaped moulds in order to obtain a second physical
PFA-pulverized fly ash;
barrier (a cement container) for tritium waste (Fig. 1).
● Cement type 2: based on cement CEM I substi-
tuted with 50% ZPb-primary lead slag (prepared
II.B. Tritium Waste
in the laboratory);
● Cement type 3: based of cement CEM I substi- Two types of solid tritium radioactive waste with
tuted with 20% CRT-cathode ray tube waste glass known tritium activity have been prepared: one type
(prepared in the laboratory).3 containing a stable hydrophilic tritium compound and
The mixes had various water-cement ratios (W/C) the other one a stable hydrophobic tritium compound.
from 0.3 to 0.5 using the same sand particle size Small pieces of paper, cotton, rubber and glass
distribution. (2–3 mm size) were contaminated with the same
The premise of the grout composition choice was known activity of tritium solution (Testosterone-1,2-T,
based on the reactive potential of pozzolana additions, specific activity = 2,1 TBq /mmol or Thymidine
which lead to hydro silicate gels during curing time. The metil-T, specific activity = 0.99 TBq/mmol). The tri-
supplementary hydrosilicate gels decrease pore volume tium activity in each waste was: 0.32 MBq/sample and
and adsorb the tritium.4 respectively, 10.2 MBq/sample.
The main compositional parameters are shown in
Table I. II.C. Tritium Immobilizations in Grout Mixtures
The grouts curing (28 days minimum) have shown com-
pact and structural integrity without pores and cracks, so as to The solid tritium waste was mixed with grout paste (mass
ensure radioactive tritium waste immobilization/ ratio: grout/waste = 50 g/2 g). The grout paste containing
encapsulation. tritium waste was casted into 2.0 cm-diameter cylindrical

TABLE I
Grout Mixes Compositional Parameters

Cement/Sand Unit Weight Marsh Flow

Grout Code Ratio Cement Type (kg/m3) Time (s) W/C Ratio

BR7 2:1 Type 1 2017 43 0.50

Z5N 1:1 Type 2 2174 56 0.30
G3 1.1 Type 3 2236 89 0.35

FUSION SCIENCE AND TECHNOLOGY · VOLUME 71 · APRIL 2017

288 FUGARU et al. · LEACHING TESTS OF THE TRITIUM WASTES IN CEMENT MIXTURES
plastic molds with a height of 4.0 cm or have been used to fill
the cement container to prepare six types of radioactive grouts
with cement matrix specimens: BR7O, Z5NO, G3O which
encapsulate waste containing hydrophilic tritium compound
and BR7A, Z5NA and G3A for waste containing hydropho-
bic tritium compound.
After the solidification, the samples were immersed
into an aqueous solution.
II.D. Leaching Test
All the prepared radioactive specimens were main-
tained for 5 days before removing the molds and then left
in a laboratory at room temperature (20 ± 2°C) and 30%
relative humidity for 40 days to develop the cementitious
matrix strength structure. The specimens were not left in
100% relative humidity in order to simulate real condi-
tions of grouts applications. The tritium waste immobi-
lized in the grout mixtures and containers made of
cementitious grout filled with tritium waste were
immersed into an aqueous solution in closed vessels.
Leaching tests were performed according to the standard
method. The sample surface to immersion liquid ratio
was >10. The tritium labeled compounds activity content
in the immersion water was measured by using a Tri-Carb
Liquid Scintillation Analyzers; Models 2300TR, Packard
Instrument Company. A predetermined volume of the
leaching solution was withdrawn at certain time intervals
and mixed with a calculated amount of scintillation liquid
and left for stabilization before counting.
III. RESULTS
The fresh grouts were characterized in terms of den-
sity and flowability. The bulk density of the grouts was
determined by using a known volume vessel.
The method used to measure grout flowability was
based on the flow cone (Marsh funnel) test according to
ASTM-C939 (Ref. 5).
TABLE II
Grout Physical Properties
Grout Code Density (kg/m3) Water Absorption (%)
BR7 2210
Z5N 2445
G3 2320
Grout mixes in hardened state were monitored for
shrinkage and mechanical strengths. The prisms of
4 × 4 × 16 cm were used for mechanical strengths and
shrinkage testing.
The shrinkage variation (mm/m) after 28 days was
−0.5 for BR7 and Z5N grout types and −1 for G3 grout
type.
The physical properties of grouts after 28 days are
presented in Table II.
The grout compressive strength and shrinkage are
considered acceptance criterions for secure LLTW
encapsulation.
The leaching of tritium from samples immersed in an
aqueous solution, expressed as percentage of the initial
tritium activity of the sample released in the immersion
liquid, has been investigated at room temperature
(25 ± 5°C) and the results are presented in Table III.
Leaching of the tritium, expressed as percentage of
the initial tritium activity of the sample released in the
immersion liquid, from LLTW solidified in grouts and
encapsulated in a cement container was also investi-
gated and the results are shown in Table IV.
IV. CONCLUSION
As can be observed from the results, the leaching
behavior of the LLTW solidified under examination
shows a pattern that could be divided into two regions.
The first region represents the initial rapid release of tri-
tium within the first 30 days, and then the drastic reduction
that took place over a long period of time where the
controlling process may be a diffusion mechanism.
The amount of tritium released from solidified grout
waste during the leaching process increased with the
leaching duration and depended on the grout type used
as solidification matrix and tritium waste composition.
The tritium trapping capacity of the grout paste type
BR7 was much larger than the trapping capacity of the
other two grout types (Z5N and G3).
Bending Strength Compressive Strength
(MPa) (MPa)
5.85 11.7 44.7
5.65 9.9 70.8
2.99 10.8 59.8
FUSION SCIENCE AND TECHNOLOGY · VOLUME 71 · APRIL 2017
 LEACHING TESTS OF THE TRITIUM WASTES IN CEMENT MIXTURES · FUGARU et al. 289

TABLE III
Value of the Tritium Activity Leached from LLTW Solidified in Different Grout Mixtures

Tritium Leaching (%)

Sample 1 day 2 days 7 days 30 days 120 days

BR7O 0.9 3.1 5.1 8.2 10.2

BR7A 1.5 5.8 8.3 12.5 15.3
Z5NO 4.1 9.7 12.2 22.5 30.5
Z5NA 7.2 14.3 26.3 37.3 42.3
G3O 3.3 7.9 10.1 22.8 25.7
G3A 4.2 9.6 12.5 18.4 20.6

TABLE IV Acknowledgments
Value of the Tritium Activity Leached from the Tritium Waste
Solidified in Different Grout Mixtures and Encapsulated in This work was performed by Partnerships Programme in
Cement Container (Grout Type BR7) priority areas -PN II, developed with the support of MENCS -
UEFISCDI, contract no. 234/2014.
Tritium Leaching
Sample (%) Time

BR7O <0.02 6 months References

BR7A <0.03
Z5NO <0.1
1. “Behaviour of Cementitious Materials in Long-Term Storage
Z5NA <0.2
and Disposal of Radioactive Waste,” IAEA-TECDOC-1701,
G3O <0.03
G3A <0.03 International Atomic Energy Agency (2013).
2. R. O. ABDEL RAHMAN et al., Cementitious Materials for
Nuclear Waste Immobilization, ISBN: 978-1-118-51200-5,
Wiley, Chichester (2015).
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grout type BR7 is leach resistant, so the release of tions and conformity criteria for common cements” (2011).
tritium from the radioactive waste will be slow even 4. N. SACA et al., “Experimental Models of Grout Type
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and is best suited to be used for immobilization of the Level Radioactivity Wastes Encapsulation,” Rom. J. Mat.,
solid tritium waste. 46, 1, 34 (2016).
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chemical as well as physical immobilization of the tritium Aggregate Concrete (Flow Cone Method),” ASTM-C939,
solid waste. ASTM International (2009).

FUSION SCIENCE AND TECHNOLOGY · VOLUME 71 · APRIL 2017