High Cesium Concentrations in Groundwater in a Coastal Granitoidic Fracture Network
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1 High Cesium Concentrations in Groundwater in a Coastal Granitoidic Fracture Network Frédéric Mathurin H. Drake, B. Kalinowski and M. Åström NGL ANNUAL SCIENCE MEETING 2014 Session 1: Deep subsurface research Physical-chemical sciences and engineering
2 Data access to the uniquely well-characterized surrounding area of Ävrö- Simpevarp-Laxemar SICADA database with more than 400 million observations
3 1. Why is natural Cs of interest in groundwater? 2. How much are the dissolved Cs concentrations? 3. How to explain the high dissolved Cs concentrations? 4. What are the direct implications?
4 Deep geological disposal of radioactive nuclear waste Crystalline rocks are considered as favorable host medium : - relatively easy to excavate - mechanical stability of the rock after underground opening - thermal properties of the bedrock (e.g. thermal conductivity) Geologically stable but: - sparsely fractured - groundwater flow in open fractures
5 Engineered barriers (KBS-3 concept) Triple barriers composed of : - (1) Copper canister - (2) Buffer layer (bentonite) - (3) Rock (geosphere)
6 Cs in a context of nuclear waste disposal Context - Retention properties of the geosphere - Cs radionuclides: 135 Cs, 137 Cs - Natural concentration of dissolved Cs: 133 Cs
7 1. Why is natural Cs of interest in groundwater? 2. How much are the dissolved Cs concentrations? 3. How to explain the high dissolved Cs concentrations? 4. What are the direct implications?
8 Area of study
9 Cs concentration in groundwater a Guillardet et al, 2003 b Faure, 1998 c Frengstad, 2000 d Bank et al, 1995 High natural Cs concentration in low temperature (<20 C) and fractured granitoidic groundwaters
10 1. Why is natural Cs of interest in groundwater? 2. How much are the dissolved Cs concentrations? 3. How to explain the high dissolved Cs concentrations? 4. What are the direct implications?
11 1. Why is natural Cs of interest in groundwater? 2. How much are the dissolved Cs concentrations? 3. How to explain the high dissolved Cs concentrations? - Origins of groundwater in the fracture network 4. What are the direct implications?
12 Tunnel influence : groundwater mixing Mathurin et al (2012) Environ Sci Technol Deep saline groundwater Modern Baltic Sea Glacial meltwater Thoroughly mixed groundwater Meteoric water
13 Influence of groundwater origins on dissolved Cs abundance Groundwater classification based on Cl and δ 18 O Cs strongly correlated with the dominant origin of groundwater Highest concentrations occur in deep saline and marine groundwaters
14 Influence of groundwater origin on dissolved Cs abundance Overall increase of Cs with the salinity Related to the residence time of groundwater Marine groundwater : - salinity of the modern Baltic Sea - Low Cs concentration in the local Baltic Sea Modern meteoric recharge High Cs concentration in groundwater: internal sources
15 1. Why is natural Cs of interest in groundwater? 2. How much are the dissolved Cs concentrations? 3. How to explain the high dissolved Cs concentrations? - Origins of groundwater in the fracture network - Cs in fracture minerals 4. What are the direct implications?
16 Fracture coating minerals - Water conductive fractures - Fracture surface of drilled cores - Chemical analyses of fracture coating
17 Cs in fracture coating minerals
18 1. Why is natural Cs of interest in groundwater? 2. How much are the dissolved Cs concentrations? 3. How to explain the high dissolved Cs concentrations? - Origins of groundwater in the fracture network - Cs in fracture minerals - Cations exchange as mechanism for high dissolved Cs concentrations in marine groundwater? 4. What are the direct implications?
19 Solute transport modelling in a dual porosity fracture: conceptual model Modeling of baltic Sea intrusion with composition of porewater from the Sea sediment (NH 4 and K rich): - - Mixing (various % dillution) - - Cation exchange (10% illite minerals in fractures) - - Selectivity coefficients taken from Bradburry and Bayens (2000)
20 Modeling results Modeling of baltic Sea intrusion with composition of porewater from the Sea sediment (NH 4 and K rich): The predicted effect of cation exchange on abundance of dissolved Cs results in substantial increase of the metal concentration Predicted exchanges in the gouge filling porosity maintain high Cs dissolved concentration in the inflowing marine groundwater during several decades
21 1. Why is natural Cs of interest in groundwater? 2. How much are the dissolved Cs concentrations? 3. How to explain the high dissolved Cs concentrations? 4. What are the direct implications?
22 Implication for risk assessment Regarding the NGL/SKB (SICADA) database: The database from the long term monitoring program is ideal to use in terms of : - assessment of the sources and controls of Cs in this setting. - estimation of the sensitivity of the retention properties of the bedrock fractures to the composition of the groundwater. In the context of risk assessment (SKB interests): - field measurements and modeling results predict that desorption can control the Cs + mobility in fracture groundwater. - retention properties of the bedrock for Cs are possibly reduced in hydraulically transmissive fractures, where marine groundwater (high K and NH 4 concentration) has recently intruded.
23 Acknowledgements Co-authors and collaborators: Funding: Swedish Nuclear Fuel and Waste Management Company (SKB), Stockholm. Thank you! Questions?
24 Summary 1. High natural Cs concentrations in low temperature (<20 C) and deep groundwaters - deep saline groundwater (up to 6 μg L -1 ) - marine groundwater (up to 6 μg L -1 ) 2. Internal source of Cs: clay rich fracture minerals including illite (>50ppm) 3. Deep saline groundwater: dissolved Cs concentrations increase with salinity and thus residence time 4. Modern Baltic Sea: reactive transport modeling (intrusion of marine water) suggests that cation exchange in the gouge fillings and reversible diffusion in the mobile pore water zone increase rapidly and persistently the dissolved Cs abundance for several decades 5. Retention property of the bedrock for Cs is possibly reduced in hydraulically transmissive fractures, where marine groundwater (high K and NH 4 concentration) has recently intruded.
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