Dmitri Bugai Institute of Geological Sciences (IGS), Kiev, Ukraine

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Groundwater contamination following the Chernobyl accident: overview of monitoring data, assessment of radiological risks and analysis of remedial measures Dmitri Bugai Institute of Geological Sciences (IGS), Kiev, Ukraine 12 December 8 September 2012, 2014, ISTC/STCU IAEA TM Technical on Groundwater Working contamination Group Meeting, following MEXT, Fukushima Tokyo accident, Vienna

Outline Introduction: Sources of groundwater contamination, Chernobyl Site hydrogeology Overview of groundwater monitoring data Review of post-accident remedial measures Risks from groundwater contamination Natural attenuation process in groundwater (data from 2001-2010) Lessons learned (having in mind Fukushima Daiichi Accident) 2

1.1 Terrestrial contamination by 137 Cs in the vicinity of ChNPP 3

1.2 Sources of groundwater contamination Radiologically important Chernobyl contaminants are: cesium-137, strontium-90, plutonium-239, 240, and americium-241 Strontium-90 has shown highest mobility in soils and groundwater; intensive migration to groundwater became evident in 1988-1989 Main sources of groundwater contamination: Radioactive fallout ( diffused source ) Sarcophagus (damaged Unit 4 of ChNPP) Radioactive waste dumps ( Red Forest ) Cooling pond of ChNPP Strontium-90 concentrations in groundwater In the near zone of ChNPP in 1998 [data of IGS] 4

1.3 ChNPP site hydrogeology Geological cross-section of Chernobyl Exclusion Zone [A.Matoshko, 1999] Hydrogeology conditions in Chernobyl zone generally favor radionuclide migration to groundwater: Humid climate (annual precipitation ~600mm) Flat landscape Local sandy deposits have relatively high permeability and low adsorption capacity; soils are slightly acidic 5

Specific activity, Bq/l 2.1 Groundwater contamination cause by diffused pollution of the ChNPP Site by radioactive fallout Typical ranges of radionuclide activity in groundwater at ChNPP Site: 90 Sr - n*10 n*0.1 Bq/l Groundwater monitoring data for well no.14-iii ( Kompleksny Site; 1988-2001) ) [EcoCenter data] 100.00 137 Cs - n*0.1-0.01 Bq/l or less 239,240 Pu - n*0.001 Bq/l or less 10.00 Cs-137 Sr-90 1.00 0.10 0.01 11.8.87 7.5.90 31.1.93 28.10.95 24.7.98 19.4.01 Date Groundwater monitoring data for well no.k-5 ( Nefebaza Site; 1990-2001) [EcoCenter data] 6

3.2 Groundwater contamination in the vicinity of Sarcophagus 137 Cs, Bq/L 90 Sr, Bq/L Maximum radinuclide concentrations in groundwater [NNC, 2001] 90 Sr - 3800 Bq/l 137 Cs - 200 Bq/l 239,240 Pu - 7 Bq/L High 137 Cs activity in groundwater can be related to leakage of highly contaminated cesium enriched water ( 137 Cs activity of ~ 0.1 50 MBq/L) from the basement premises of Sarcophagus 7

ChNPP site map 3.3 Experimental site (EPIC) at Red Forest waste dumps (IGS UIAR IRSN, 2000-2012) monitoring data CHERNOBYL database Pit for unsaturated zone monitoring Pit (UZ) monitoring well cluster 8

3.4 Elements of monitoring system at EPIC site in Chernobyl Red Forest On-site laboratory module Station for unsat. zone monitoring Monitoring wells Meteorological station 9

3.5 Groundwater contamination at Red Forest waste dump site 90 Sr distribution in the aquifer cross-section at Trench no.22 (2002) Infiltration rate 200-250 mm/y groundwater flow velocity ~10 m/y In-situ 90 Sr retardation factor: R~ 14 (7% of GW flow velocity) 90 Sr Kd values from field tests: 0.5-2 L/kg (for eolian sand deposits) 10

3.6 137 Cs migration behavior in soils and groundwater Regional groundwater monitoring system in Chernobyl zone usually reports 137 Cs concentrations of n 0.01 - n 0.1 Bq/L In general 137 Cs shows low mobility in mineral soils of Chernobyl zone 137 Cs concentrations in groundwater of Red Forest ranged within n 0.1 - n 1 Bq/L 137 Cs sorption Kd-s from lab batch tests are 100-170 l/kg ; 137 Cs retardation factor from column test is R=6600 [S.Szenknect 2003] Main factors controlling 137 Cs migration in soil profile: - radionuclide fixation by clay minerals, sorption by ionexchange; - biogeochemical RN cycling in soil plant system; - water regime of soils; - radioactive decay Dynamics of ionexchangeable forms of 137 Cs in soddy-podzolic soils followin Chernobyl accident Effective half-life for fixation T ½ is 0.8 1.4 years (first 5 y) [Ivanov and Kashparov, 2003] 11

4.1 Post-accident groundwater remedial measures Governmental Decree on groundwater protection measures was adopted on 30 May 1986 Urgency of remedial measures was dictated by the potential threat from the hydrological river transport of fall-out radionuclides to the Ukrainian capital Kiev and other downstream populations (9 million pers. using Dnieper water); One other concern was protection of local water supply wells (exploiting the Eocene aquifer) 12

5.2 Lessons from inefficient emergency remedial measures Groundwater remedial measures were based on incomplete knowledge and the worst case analysis ( assumed maximum solubility of fallout; maximum fallout densities; minimal retardaiton ) Based on monitoring data and updated radioctivity survey data by the end of 1986 the groundwater remediation projects were stopped. Only 2.2 km of the initially planned 8.5km of the slurry wall barrier were completed. The protective drainage systems were put on reserve (the equipment being later dismantled) Project design of a slurry wall around ChNPP [Spichak, 1999] The payment for overconservative remedial assessments were: - High and unnecessary remediation costs ( e.g., cooling pond drainage system cost was 22 mill.rubles); - unnecessary exposures to mitigation workers(the exposure rates at ChNPP in the summer period of 1986 were about 0.001 0.01 Sv/h). Mistakes in emergency remedial measures resulted from: - lack of reliable radiological information and assessment models; - absence of criteria for decision making regarding a need for remediation; - absence of peer review by independent experts 13

6.1 Risks caused by groundwater contamination Off-site risks Projected max. 90 Sr release rate from the ChNPP Site is approx. ~0.1 TBq /y or 0.02% per year from initial watershed inventory Sufrace water r transport of 90 S (~10-20 TBq/y in 1989-1991) was dominated by wash-off of radionuclides from floodplains and from wetlands Water pathway contributed only 6% of dose to the resident of Kiev Region (in 1993); doses induced by water pathway are estimated at 10-2 - 10-3 msv/y [Berkovsky et al., 1993] Screening forecast of 90 Sr transport from sources at ChNPP Site [Bugai et al., 1998] On-site risks On-site radilogical risks for hypothetical residents in Chernobyl Zone are dominated by risks caused by surface contamination [Bugai et al., 1996] Probabilistic analysis has shown low risk of contamination of water wells exploiting Eocene aquifer [Bugai and Smith, 1996] 14

6.2 Modeling predictions of 90 Sr in groundwater transport from Sarcophagus [Kivva, Zhelaznyak, 1997] t=100 y t=1000 y 15

6.3 Modeling predictions of 90 S transport in groundwater from Red Forest waste dumps [Bugai tal., 2012] Predicted long-term 90 Sr transport in the aquifer from Trench no.22 at Red Forest Site Modeling results: the maximum distance of 90 Sr migration from the waste site in conc. >2 Bq/L ( 90 Sr drinking standard in Ukraine) constitutes 200 m; The aquifer is contaminated to the depth of about 15 m; In about 250 a 90 Sr concentrations throughout the aquifer will decrease below 2 Bq/L Conclusion: Red Forest waste site does not pose risk of contamination of Pripyat River 16

6.4 Water protection measures in Chernobyl zone in 1990-2000 Based on prioritization of contaminant sources and modeling analyses, in later period (1990-2000) water protection measures focused on isolation of flood plain areas of Pripyat River in the vicinity of ChNPP contaminated by fallout radionuclides Protective dikes isolating contaminated floodplain areas of Pripyat River in the near zone of ChNPP The current recommended strategy for contaminated groundwater is monitored natural attenuation (MNA) 17

NO3, mg/l 90Sr, Bq/l 7.1 Natural attenuation process in groundwater : Geochemical regime of the aquifer at Red Forest waste dump site Mean 90 Sr plume concentration 1997-2001 Mean 90 Sr plume concentration 2002-2008 2000 1800 1600 Increase of 90Sr caused by flooding by groundwater of trench bottom in May- June 2005 1400 1200 Radioactive decay line 1000 800 Linear trend in monitoring data 600 400 200 0 04.01 02.02 12.02 10.03 08.04 05.05 03.06 01.07 11.07 09.08 Mean NO 3 plume concentration 2004-2008 Mean Ca plume concentration 1998-2002 50 45 40 35 30 25 20 15 10 5 0 09.04 03.05 09.05 03.06 09.06 03.07 09.07 03.08 09.08

7.2 Conceptual bio-geochemical radionuclide migration model for the Red Forest waste dump site 90 Sr fluxes from the trench: Biogenic flux: 0.82% a -1 from trench inventory in 2005 [Thiry et al., 2009] Geo-migration 0.14-0.5% a -1 (1987-2000) [Bugai et al., 2001] Ref: A Martin-Garin, NVan Meir, C Simonucci, V Kashparov, D Bugai Quantitative assessment of radionuclide migration from near-surface radioactive waste burial sites: the waste dumps in the Chernobyl exclusion zone as an example, In: Radionuclide behavior in the natural environment, Woodhead Publishing, 2012

7.3 Natural attenuation process in groundwater of Red Forest Evolution of 90 Sr migration fluxes from trench no.22t in 1988-2008 Biogenic factors contributing to natural attenuation in GW: - direct RN uptake by vegetation and incorporation to biological cycle; - nutrient element (Ca,K ) uptake by vegatation, which influences GW geochemistry and hence - RN mobility 20

8.1 Lessons learned (assessment of risks and remedial planning) Assessment for remedial activities must use realistic analyses and incorporate best science Remediation criteria and objectives should be clearly defined early in the assessment phase of groundwater remedial activities. Groundwater contamination problems should be considered within the big picture of various radionuclide exposure pathways and risks ( Decision-makers and ordinary public often suppose that groundwater contamination entails much higher risk than it really does) A peer review of proposed actions is important Adequate modeling of long-term radioactive contaminant transport in unsaturated zone and groundwater requires integrated ecosystem approach 21

8.2 Chernobyl lessons learned: Diagram of the terrestrial radioecological model knowledgebase components THANK YOU FOR YOUR ATTENTION! 22