『Abstract
This work, which was done within the Swedish nuclear waste management
program, was carried out in order to increase the understanding
of the mobility and fate of rare earth elements (REEs) in natural
boreal waters in granitoidic terrain. Two areas were studied,
Forsmark and Simpevarp, one of which will be selected as a site
for spent nuclear fuel. The highest REE concentrations were found
in the overburden groundwaters, in Simpevarp in particular (median
ΣREE 52μg/L), but also in Forsmark (median ΣREE 6.7μg/L). The
fractionation patterns in these waters were characterised by light
REE (LREE) enrichment and negative Ce and Eu anomalies. In contrast,
the surface waters had relatively low REE concentrations. They
were characterised either by an increase in relative concentrations
throughout the lanthanide series (Forsmark which has a carbonate-rich
till) or flat patterns (Simpevarp with carbonate-poor till), and
had negative Ce and Eu anomalies. In the bedrock groundwaters,
the concentrations and fractionation patterns of REEs were entirely
different from those in the overburden groundwaters. The median
La concentrations were low (just above 0.1μg/L in both areas),
only in a few samples were the concentrations of several REEs
(and in a couple of rare cases all REEs) above the detection limit,
and there was an increase in the relative concentrations throughout
the lanthanide series. In contrast to these large spatial variations,
the temporal trends were characterised by small (or non existent)
variations in REE-fractionation patterns but rather large variations
in concentrations. The Visual MINTEQ speciation calculations predicted
that all REEs in all waters were closely associated with dissolved
organic matter, and not with carbonate. In the hydrochemical data
for the overburden groundwater in particular, there was however
a strong indication of association with inorganic colloids, which
were not included in the speciation model. Overall the results
showed that within a typical boreal granitoidic setting, overburden
groundwaters are enriched in REEs, organic complexes are much
more important than carbonate complexes, there is little evidence
of significant mixing of REEs between different water types (surface,
overburden, bedrock) and spatial variations are more extensive
than temporal ones.』
1. Introduction
2. Method
2.1. Study area
2.2. Sampling
2.3. Analyses
2.4. Speciation
2.4.1. Model description
2.4.2. Optimization of metal binding parameters for the SHM
2.4.3. Model application
3. Results
3.1. Bedrock groundwater
3.2. Overburden groundwater
3.3. Stream water
3.4. Lake water
4. Discussion
4.1. General patterns
4.2. Speciation
4.3. Controls of abundance
4.4. The redox sensitive metals
4.5. Actinide analogues
5. Conclusions
Acknowledgements
References