Supplementary data
Plutonium partitioning in three-phase systems with water, granite grains,
and different colloids
Jinchuan Xie*, Jianfeng Lin, Xiaohua Zhou, Mei Li, Guoqing Zhou
Northwest Institute of Nuclear Technology, P.O. Box 69-14, Xi’an City, Shanxi Province 710024, PR
China
* Corresponding author, Tel.: +86 29 84767789, fax: +86 29 83366333.
E-mail address: xiejinchuan@hotmail.com.
Chemical constituents of the granite and soil samples
Table S1 Elemental composition of the granite
Composition
Mass content %
SiO2
Al2O3
FeO
Fe2O3
K2O
Na2O
CO2
MgO
CaO
65.2
15.6
3.74
0.60
3.59
2.70
2.51
2.07
1.99
Composition
Mass content %
H2O
1.10
TiO2
S
SO3
P2O5
MnO
U
Ta
0.52
0.41
0.047
0.24
0.15
1.85 (ppm)
0.70 (ppm)
Table S2 Elemental composition of the soil
Composition
Mass content %
SiO2
Al2O3
CaO
Fe2O3
MgO
K2O
Na2O
TiO2
MnO
Ignition loss
60.5
10.4
8.95
3.55
3.25
2.37
2.04
0.44
0.10
8.4
0
-5
-10
Zeta potential (mV)
Zeta potential (mV)
0
-10
-15
-20
-30
-20
-25
0.0
0.1
0.2
0.3
0.4
0.5
Soil colloids
-40
Colloidal granite particles
0.0
0.6
0.1
0.2
0.3
0.4
0.5
0.6
+
Na concentration (mol/L)
+
Na concentration (mol/L)
a
b
Fig. S1 Zeta potentials of the colloidal granite particles (a) and the soil colloids (b) with the diameters of
< 1 μm, responded to the variation in Na+ concentration. These two experiments were performed under
the environmentally relevant pH 8.5 conditions.
The flow diagram for determination of the Pu oxidation state distribution
Colloidal
suspension
Remove 2.5ml for
10 kD ultrafiltration
Filtrate
a
Acidify remaining colloids to pH
1.5 using 1M HClO4 for 3 min
Remove 0.5ml from filtrate a
or b for ICP-MS counting
10 kD ultrafiltration
Pu(IV
)
Filtrate
b
Elute with 20ml of
8M HNO3 for 20min
at 150-200℃
Total Pu for
filtrate a and b
×5
Centrifuge
at 4350g
Solvent extraction oxidation analysis
(Analysis of a and b performed independently)
Add 0.7ml filtrate to 0.3ml 3.3M HNO3 and
shake with 1.0ml 0.5M TTA for 5 min.
Residual for
colloidal solid
Add 0.7ml filtrate to 0.3ml 3.3M HCl and
shake with 1.0ml 0.5M HDEHP for 10 min.
Supernatant
Heated to near dryness
Aqueous phase
Pu(V),Pu(VI)
Remove 0.5ml
for ICP-MS
counting
Organic
phaes Pu(IV)
Organic phaes
Pu(IV),Pu(VI)
Aqueous
phase Pu(V)
2% HNO3
ICP-MS
Remove 0.5ml
for ICP-MS
counting
Fig. S2. The analytic flow diagram used to determine the distribution of Pu oxidation state, IV, V and VI.
This technique was initially employed by Keeney-Kennicutt and Morse (1985), subsequently modified by
Morgenstern and Choppin (2002) and Powell et al. (2004), and further improved to measure 239Pu
concentrations by ICP-MS in this study.
References:
Keeney-Kennicutt WL, Morse JW (1985) The redox chemistry of Pu(V)O 2+ interaction with common mineral
surfaces in dilute solutions and seawater. Geochim Cosmochim Ac 49:2577-2588
Morgenstern A, Choppin GR (2002) Kinetics of the oxidation of Pu(IV) by manganese dioxide. Radiochim Acta
90:69-74
Powell BA, Fjeld RA, Kaplan DI, Coates JT, Serkiz SM (2004) Pu(V)O 2+ adsorption and reduction by synthetic
magnetite (Fe3O4). Environ Sci Technol 38:6016-6024