nuclear test plutonium and radiocaesium dispersion …nuclear test plutonium and radiocaesium...
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Nuclear test plutonium and radiocaesium dispersion in lakes ecosystems: experimental data and novel modelling approach T1.3-P11
A. Puzas*, D. Baltrūnas, E. Maceika, B. Lukšienė, V. Filistovič, N. Tarasiuk, E. Koviazina, M. Konstantinova, Š. Buivydas
Institute of Physics of Center for Physical Sciences and Technology, LITHUANIA *[email protected]
Problem
Commonly, migration of the
technogenic radionuclides from water into soil
and bottom sediments in the natural
environment is described by one-stage models.
The main drawback of such models is related
to the fact that the radionuclide diffusion
coefficient in sediments decreases with time.
However, analyses of radionuclide
vertical profiles in carbonate bottom sediments
as well as results of laboratory experiments
show that the process proceeds in two
temporal stages. The first fast migration stage
is governed by the light ion transfer. The
resulting vertical profile of the radionuclide
activity concentration in sediments is
exponentially decreasing with depth. The
second migration stage is slow. It involves the
main significant processes: bioturbation,
sedimentation as well as the first order kinetic
reactions and radioactive decay.
In the case of accidental appearance
of radionuclides in water systems the one-
phase model cannot be properly employed to
predict the long-term consequences of
radionuclide migration into zones where they
are mostly accumulated - bottom sediments
and soil solid phase. Application of the correct
model of radionuclide behavior in the
radioactive waste storage environment and in
water saturated soils is of great concern as
well.
Solution
The two-phase mathematical model of
the radionuclide vertical migration in the water
saturated solids (bottom sediments and soil).
There is considered process of slow
sorption and desorption of the radionuclide
mobile fraction by solid particles.
Transport of the radionuclide in the two-phase
environment is described by 1-D advection-
diffusion equations, separately for the liquid
volumetric activity c and flux- j(c), and solid
phase specific activity cs and flux- js(cs) :
fsecct
j
ccc vDj
sfssbsbsb ecct
j
sssss ccc vDj
ssffs cce
Where: f – rate of activity transfer
from liquid to solid phase in the
sediments [d-1],
s – rate of the transfer from
the solid to the liquid phase [g cm-3 d-1].
sb 1
Radioactive contaminant
activity vertical distribution profile
is considered as a process having
two stages (I and II):
• the first stage (I) is
related with the migration
of the contaminant from
water to the
sediments,
• whereas, the second
stage (II) – with the further
transformation of the
deposited contaminant.
ccx
cv
x
cD
xt
c f
vols
b
s
,
vols
b
ssfvols ccc
t,,
Advection-diffusion equations for
the liquid volumetric activity c and
solid phase volumetric activity cs,vol :
Boundary conditions for the stage (I) :
tgvx
txcDtxvc ee
x
exp1,
, 0
0
0
,
xx
txc
0,0
ttxc 0,
0
ts txc 0,0,
tvols txc
Advection-dispersion,
degradation and non-equilibrium
exchange between phases during
the stage (I) together with the
boundary conditions and zero
initial conditions belongs to the
boundary value problem (BVP)
solution.
0
X
TC ,
Stage (I)
Initial conditions for the stage (I) :
0 5 10 15 20 25 30 10
-4
10 -3
10 -2
10 -1
10 0
10 1
Sediment depth, cm
Activity c
on
ce
ntr
ation
,
Bq
cm
-3
Red line -
Liquid
Dark line –
Solid
Dot line T=100
days
Solid line
T=200 days
dXGwaTww
aTV
dXGwaTww
aTVTXC
T
E
RR
R
T
R
,,,;expexpexp
,,,;expexpexp,
212
0
0
212
0
0
dXGwaTww
a
w
TV
dXGwaTww
a
w
TVTXC
s
T
f
RR
RR
s
T
fs
,,,;exp1exp1
exp
,,,;exp1exp1
exp,
222
0
0
222
0
0
X
XX
X
X
P
XerfcXP
P
P
XPXG
/exp
/expexp,
424
2
1 1
1
222
1
1
n
n
k
knn
k
k
kn
T
n
a
wTwa
!!,,;
1 1
221
1
n
n
k
knn
k
k
kn
T
n
a
wTwa
!!,,;
fsa 2
sEw
sRRw
As a result of the stage (I) solution
we receive vertical distribution of the
radionuclide activity profile, depending
on depth for the liquid phase
f1(X)=С(Tmax,X) and for the solid phase
f2(X)=Сs(Tmax,X). Duration of the stage (I)
Tmax should be long enough, to reach
activity flux equilibrium between water
and sediments.
0
0
gvx
cDcv r
x
xfxfxc EE 1110 ,, exp,
xfxfxc EEs 2220 ,, exp,
Stage (II)
Profile of the contamination distribution,
obtained from the stage (I), is used as an
initial conditions for calculating the solution of
the two phases concentration distributions in
the stage (II).
Boundary conditions for the stage (II) :
Initial conditions for the stage (II) :
0
,
xx
txc
0 20 40 60 80 100 0
0.01
0.02
0.03
0.04
0.05
0.06
0.07
0.08
Sediment depth, cm
Activity c
on
ce
ntr
ation
,
Bq c
m-3
Red line -
Liquid
Dark line –
Solid
Dot line
T=5000 days
Solid line
T=10000 days
dXGTHT
afXGTHf
TXGfTXC
T
EEEsE
EE
0
1212
12202
121
,,,,
,,
;,,;,,
;,,
dXGTHTa
fdXGTHf
TXfTXC
T
E
T
EEE
sEEs
0
221
0
221201
22
,,,,
,,
;,,;,,
exp,
TaITTH nsn 22exp, (n = 0, 1)
X
XX
X
XX
X
X
X
X
P
XerfcXP
P
P
PXerfcXP
P
P
PXerfcX
PXG
22
2
211
2
1
2
21
2
11
2
2
exp
exp
exp
exp;,
In(x) – is modified the nth order Bessel function of
the first kind, erfc(x) – error function complement.
Integrals are solved numerically by using
Chebyshev–Gauss quadrature method.
Where:
Where:
Measurements
Lake Juodis, located near Vilnius city, Lithuania
Parameter Value
Parameters for stage I
L – Length of the sediment layer 100 cm
v – Darcy velocity 0.008 cm day-1
D – dispersion (diffusion) coefficient 0.2 cm2 day
-1
s –sediment dry matter density 1.0 g cm-3
b –sediment balk density 0.043 g cm-3
= 1 - b / s – porosity 0.96
kD – exchangeable part KD 500 cm3 g
-1 or L kg
-1
12 f – exchang. part velocity f = ln(2)/20 = 0.0347 day-1
21 s – exchang. part velocity s =f / (kD*b) = 0.0016 day-1
f – degradation (decay) constant ln(2) / (30*365.25) = 0.000063 day-1
s – degradation (decay) constant 0.000063 day-1
ge – initial water activity in Lake 1.0 Bq cm-3
e – activity decrease in Lake const. ln(2) / 30 = 0.023 day-1
v0 – activity deposition rate in Lake water 0.1 cm day-1
Additional parameters for stage II
fe1 – initial activity at x=0 (water ph.) 0.697 Bq cm-3
e1 – expon. decrease rate by depth 0.0807 cm-1
fe2 – initial activity at x=0 (solid ph.) 0.591 Bq cm-3
e2 – expon. decrease rate by depth 0.0875 cm-1
21 – from solid phase to water phase 0.0385 day-1
μ1 – degradation+decay+exch. const. 0.0362 day-1
12 – from water phase to solid phase 0.0346 day-1
μ 2 – degradation+decay+exch. const. 0.0369 day-1
Measured 137Cs activity in flooded soil core of the lake Juodis
Conclusion
The two stage and two phase (liquid and solid) radionuclide migration in the
water-sediments ecosystem model is suitable to be used for better prediction of the
long-term consequences of radionuclide accumulation and transport after the
accidental contamination of lake water.
Nuclear tests
Chernobyl
Fukushima
Vertical profiles of plutonium isotope activity concentrations
and activity concentration 238Pu/239,240Pu ratios in the flooded
soil core of the lake Juodis
Plutonium isotope activity concentrations and activity
concentration 238Pu/239,240Pu ratios in the sediment vertical profile
from the lake Juodis
Volumetric activities [Bq m−3] depending on the depth of
sediments x [cm] for the liquid phase of the sediments cL
(red), for the solid-phase kinetic parts cSK (blue) of the total
aggregated volumetric activities in solid phase (kinetic and
fast) cS (green) and measured volumetric activities (total
aggregated) cS,exp (points)
Simulation of 137Cs volume activities cSK and cL [Bq m−3] in
sediment solid and liquid phases, respectively, depending on
the sediment depth x [cm] and on time after the acute release
of 137Cs activity into the lake, obtained using the mathematical
model
Vertical profiles of 239,240Pu and 137Cs activity
concentrations in the sediment core taken in the lake
Juodis in July, 2012. Vertical lines indicate 137Cs/239,240Pu
ratio for the global fallout (29 ± 3 value, reference year
2012)
Volumetric activity of the kinetic part of a solid phase
and b liquid phase of sediments depending on the depth
of sediments at different equilibrium values of partition
coefficients KDS [m3 kg]
References:
1. B. Lukšienė et al. J Radioanal Nucl Chem (2014) 300:277–286
2. V. Filistovič et al. Water Air Soil Pollut (2015) 226:202