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Hanford Site Composite Analysis: Recharge and Inventory Sensitivity Analyses for the A Trenches, BC Cribs and Trenches, and PUREX Area Vadose Zone Models

The main objectives of the composite analysis (CA) compliance case vadose zone (VZ) facet are to simulate transport of radionuclide releases from the surface to the water table, and to provide radionuclide transfer rates to groundwater for inclusion into the Plateau-to-River (P2R) saturated zone (SZ) model (CP-57037, Model Package Report: Plateau to River Groundwater Model, Version 8.3). The CA compliance case approach to address the scale and distribution of contaminant sources in the VZ facet is to subdivide the Hanford Site Central Plateau into 26 models that contain contaminant sources and liquid discharges likely to commingle during migration through the VZ to the water table

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Contaminant Transport Simulation with the P2R Model for the Composite Analysis Base Case

In order to meet the requirements of U.S. Department of Energy (DOE) in DOE O 435.1, Radioactive Waste Management, a composite analysis (CA) must be completed for the Central Plateau at the Hanford Site. The updated Hanford CA requires estimates of fate and transport of radionuclides in the groundwater from multiple sources within and downgradient of the Central Plateau.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Incorporating Heterogeneity into 3D Geologic Models for the Alluvial Basin Reference Case

The unsaturated zone alluvium reference case is one of several geologic systems under consideration by the U.S. Department of Energy Office of Nuclear Energy for hosting repositories for spent nuclear fuel and associated waste (Sevougian et al., 2019). As noted by Mariner et al. (2018), the generic alluvial basin offers positive attributes that merit its consideration as a reference case by the Spent Fuel and Waste Science and Technology (SFWST) campaign. Hundreds of alluvial basins and sub-basins are scattered across the arid western United States (Figure 1-1). Precipitation and infiltration rates are relatively low with high evapotranspiration, resulting in deep regional water tables. Deep regional water tables allow for significant vertical separation between proposed repository depths and groundwater and thus longer transport paths from a hypothetical repository to an aquifer. Accumulations of alluvial sediments within these basins are typically on the order of hundreds of meters, and locally may exceed 1,000 m in thickness, as is the case for the Deming sub-basin in southern New Mexico. In alluvial basins, alluvium creates a thick geologic host medium that serves as the natural barrier system (NBS) in the conceptual model framework of a geologic disposal system and isolates the waste packages from receptors in the biosphere. Further, alluvial basin fill is typically comprised of stacked playa and lacustrine deposits along the basin axis (Perry et al., 2018). Characterized by low permeability, these layers protect the biosphere above the repository and the groundwater resources below the repository by limiting flow and transport of radionuclides.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Microbial Influence on the Mobility of +3 Actinides from a Salt-Based Nuclear Waste Repository

Biologically enhanced transport of radionuclides is one of several processes that can affect the performance of a nuclear waste repository. In this work, several microbial isolates from the Waste Isolation Pilot Plant (WIPP) were tested for their influence on the concentration of neodymium, as an analog for +3 actinides, in simple sodium chloride solutions and in anoxic WIPP brines. Batch sorption experiments were carried out over a period of 4–5 weeks. In many cases, the effect on neodymium in solution was immediate and extensive and assumed to be due to surface complexation. However, over time, the continued loss of Nd from the solution was more likely due to biologically induced precipitation and/or mineralization and possible entrapment in extracellular polymeric substances. The results showed no correlation between organism type and the extent of its influence on neodymium in solution. However, a correlation was observed between different test matrices (simple NaCl versus high-magnesium brine versus high-NaCl brine). Further experiments were conducted to test these matrix effects, and the results showed a significant effect of magnesium concentration on the ability of microorganisms to remove Nd from solution. Possible mechanisms include cation competition and the alteration of cell surface structures. This suggests that the aqueous chemistry of the WIPP environs could play a larger role in the final disposition of +3 actinides than the microbiology.

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Radionuclide tracing based in situ corrosion and mass transport monitoring of 316L stainless steel in a molten salt closed loop

In the study, we report an in situ corrosion and mass transport monitoring method developed using a radionuclide tracing technique for the corrosion study of 316L stainless steel (316L SS) in a NaCl–MgCl 2 eutectic molten salt natural circulation loop. This method involves cyclotron irradiation of a small tube section with 16 MeV protons, later welds at the hot leg of the molten salt flow loop, generating radionuclides 51 Cr, 52 Mn, and 56 Co at the salt–alloy interface. By measuring the activity variations of these radionuclides at different sections along the loop, both the in situ monitoring of the corrosion attack depth of 316L SS and corrosion product transport and its precipitation in flowing NaCl–MgCl 2 molten salt are achieved. While 316L SS is the focus of this study, the technique reported herein can be extended to other structural materials being used in a wide range of industrial applications.

36 MATERIALS SCIENCE↗

Explosive Byproduct Gas Transport Through Sorptive Geomedia

Current underground nuclear explosion (UNE) detection strategies rely heavily on atmospheric noble gas sampling of radioxenon. However, discriminating nuclear weapons testing programs from civilian sources is difficult due to highly variable atmospheric radioxenon backgrounds and processes affecting subsurface transport of parent radionuclides. Here, we aim to study the transport of gases produced by subsurface explosions as novel stable signatures for underground nuclear explosion (UNE) monitoring. These gases may be produced in large quantities with distinct molecular ratios, which will be impacted by subsurface transport processes. To demonstrate how ratios of gases produced by explosions can change during transport in geomaterials, we conducted laboratory benchtop experiments on the transport of carbon dioxide (CO 2 ) and hydrogen (H 2 ) gases through variably saturated zeolitic tuff, which is abundant at the historic US testing site. We observed that zeolitic tuff sorbs substantial quantities of CO 2 while allowing H 2 to transport more freely, leading to changes in the molecular ratios of the two gases along the transport pathway. Gas uptake in the dry zeolitic tuff core was 72.3% for CO 2 , compared with 53.4% for xenon and 7.6% for H 2 . The presence of 20% water saturation disrupted the CO 2 sorption process, though to a lesser extent than observed for noble gases, with a 36.7% drop in xenon sorption compared with a 21.9% drop for CO 2 . These results represent the first observations of zeolite sorption altering explosive gas ratios during transport through geomedia relevant to nuclear proliferation monitoring.

54 ENVIRONMENTAL SCIENCES↗

User’s Manual for RESRAD-BUILD Code V.4: Vol. 1 – Methodology and Models Used in RESRAD-BUILD Code

The RESRAD-BUILD computer code models radionuclide release and transport in indoor environments and performs pathway analyses to evaluate the potential radiological dose and risk incurred by an individual who works or lives in a building contaminated with radioactive material or housing radioactively contaminated furniture or equipment. The code provides four geometries to characterize a radiation source: point, line, area, and volume, in which radionuclides are homogeneously distributed. Radionuclides contained in a source are considered to be released to the indoor air due to various processes including erosion (mechanically or weathering), diffusion (for tritium and radon in a volume source), or emanation (radon in a point, line, or area source). The release can proceed through different time phases with different rates. In RESRAD-BUILD Version 4.0, a dynamic ventilation model is implemented to simulate the fate and transport of source material particles and radionuclides after their releases. This dynamic ventilation model considers (1) air exchange between rooms in the building and between the rooms and the outdoor environment, (2) deposition from air to floor, (3) resuspension from the floor to the air, and (4) periodical vacuuming that reduces the floor deposition. The fate and transport modeling provides estimates of radionuclide concentrations in the source, in the air, and on the floor at different times, which are then integrated over the exposure duration for the calculation of radiation doses and cancer risks. A single run of the RESRAD-BUILD code can model a building with up to 9 rooms, 10 sources, and 10 receptors. The potential radiation dose and cancer risk incurred by each receptor are calculated for seven exposure pathways: (1) external radiation directly from the sources (accounting for shielding), (2) external radiation from radioactive particles deposited on the floors, (3) external radiation from airborne radionuclides, (4) inhalation of airborne radionuclides, (5) inhalation of radon and radon progenies, (6) inadvertent ingestion of radioactive particles directly from the source, and (7) ingestion of radioactive particles deposited on the floors. Various exposure scenarios can be modeled with RESRAD-BUILD, including but are not limited to, office worker, renovation worker, decontamination worker, building visitor, and resident. Both deterministic and probabilistic analyses can be performed to obtain results in both text reports and graphic displays.

61 RADIATION PROTECTION AND DOSIMETRY↗

Vadose and Saturated Zone Flow and Transport Calculations for the Active Trenches of the Low-Level Burial Grounds, Hanford Site, Washington

The purpose of the fate and transport modeling described in this environmental calculation file (ECF) is to evaluate the impacts to groundwater associated with waste disposal operations at Mixed Waste Low-Level Burial Ground (LLBG) Trenches 31 and 34 to satisfy requirements in DOE O 435.1, Radioactive Waste Management. The model integrates the flow and transport in the vadose zone beneath the active trenches with the saturated zone downgradient of the trenches to predict the radionuclide concentration at the point of assessment (POA). DOE M 435.1-1, Radioactive Waste Management Manual, defines the POA as the point of highest projected dose or concentration beyond a 100 m (328 ft) buffer zone surrounding the disposed waste. The modeling is conducted in accordance with the DOE G 435.1, Implementation Guide for Use with DOE M 435.1-1, performance assessment (PA) guidelines. The modeling involves evaluation of the groundwater concentrations and radionuclide arrival times during the 1,000-year compliance and 10,000-year sensitivity-uncertainty periods per DOE O 435.1 and DOE M 435.1. This analysis does not consider radionuclide release during facility operations, only the post-closure impacts of the radionuclides to the environment. The evaluation of potential radiological dose to groundwater receptors caused by releases from a closed facility containing radioactive waste typically includes the following: (1) Release of radionuclides from that facility (2) Transport of those radionuclides through the environment, and (3) Exposure to humans to environmental concentration levels of those radionuclides The fate and transport three-dimensional (3D) model analysis involves the post-closure impacts to the environment of the technetium-99, iodone-129, and uranium (all isotopes in the waste). The residual inventory estimates include several radionuclides, but technetium-99 is typically responsible for almost all of the beta-gamma dose equivalent associated with groundwater (water resources) protection per 40 CFR 141, “National Primary Drinking Water Regulations” (e.g., see the results in WCH-520, Performance Assessment of Environmental Restoration Disposal Facility, Hanford Site, Washington; hereinafter referred to as the ERDF PA), and iodone-129 can also be a significant dose contributor for some waste (e.g., RPP-RPT-59958, Performance Assessment for the Integrated Disposal Facility, Hanford Site, Washington; hereinafter referred to as the IDF PA). Uranium does not typically factor significantly into the impacts to groundwater, even during the 10,000-year sensitivity-uncertainty period, but always remains of interest as a contaminant. This ECF does not address vadose and saturated zone modeling for Trench 94 of the 200 East Area LLBG. Current information confirms the validity of the low corrosion rate of the naval reactor plant carbon steel (HY-80), and the even lower corrosion rate of the nickel-iron-chromium alloy reactor vessel (Inconel Alloy 600) presented in DOE/EIS-0259, Final Environmental Impact Statement on the Disposal of Decommissioned, Defueled Cruiser, Ohio Class, and Los Angeles Class Naval Reactor Plants. Based on these low corrosion rates, the time to breach the reactor vessel to allow release of radionuclides from the activated metal of the reactor vessel internal structure is at least 10,000 years. This time to breach precludes the need to evaluate the vadose and saturated zone transport of contaminants released from the reactor compartment disposal packages in the 200 East Area LLBGs PA (CP-63826, Waste Release Model Package Report for the Active Trenches of the Low-Level Burial Grounds, Hanford Site, Washington).

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Review and Assessment of Available Data Regarding the Behavior of Sodium Aerosols

Recently, there has been a resurgence of interest in advanced (non-light water) reactor designs, including sodium fast reactors (SFRs). In parallel, multiple efforts are underway to develop risk informed, performance-based licensing pathways for advanced reactors. However, such licensing approaches depend on the accuracy of the associated safety assessments, including mechanistic source term (MST) analyses. Unlike historical source term assessments, which utilizes bounding estimates of radionuclide release, MSTs attempt to realistically estimate the transport and retention of radionuclides for specific transient scenarios. For SFR MST analyses, the behavior of radionuclide aerosols is a key factor, as noted in recent studies. Due to the use of sodium as the primary coolant, many potential transient scenarios involve the release of radionuclide aerosols in conjunction with sodium aerosols. For such scenarios, sodium may be the dominant aerosol species, compared to that of released radionuclides. Therefore, understanding the behavior of sodium aerosols is particularly important to an accurate assessment of aerosol transport. Although many approaches to aerosol modeling exist, it is vital to establish their capabilities in evaluating sodium aerosol behavior for SFR analyses.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Charging of radioactive and environmental airborne particles

The charging of various airborne particles was investigated using single-particle levitation and charge-balance equations. Though radioactive decay and triboelectrification can induce charging, it is typically assumed that the aerosols in a radioactive plume will not carry significant charge at steady state since atmospheric particles can have their charge neutralized through the capture of adjacent counter-ions (i.e., diffusion charging). Here to assess this assumption, we directly measured the surface charge and charge density of various triboelectrically charged aerosols including radioactive uranium oxide (<1 μm), urban dust, Arizona desert dust, hydrophilic and hydrophobic silica nanoparticles, and graphene oxide powders using an electric field-assisted particle levitator in air. Of these particles, uranium oxide aerosols exhibited the highest surface charge density. Charge balance equations were employed to predict the average charge gained from radioactive decay as a function of time and to evaluate the effects of diffusion charging on triboelectrically charged radioactive and non-radioactive particles in the atmosphere. Simulation results show that particles, initially charged through triboelectrification, can be quickly discharged by diffusion charging in the absence of radioactive decay. Nevertheless, simulation results also indicate that particles can be strongly charged when they carry radionuclides. These experimental and simulation results suggest that radioactive decay can induce strong particle charging that may potentially affect atmospheric transport of airborne radionuclides.

54 ENVIRONMENTAL SCIENCES↗

Unclassified Source Term and Radionuclide Data for the Groundwater Flow and Contaminant Transport Model for Corrective Action Units 101 and 102: Central and Western Pahute Mesa, Nye County, Nevada, Revision 1

This report documents the evaluation of information and data available on the unclassified source term and radionuclide (RN) contamination for Central and Western Pahute Mesa (PM): Corrective Action Units (CAUs) 101 and 102. The Central and Western PM CAUs constitute two areas of the Nevada National Security Site (NNSS) used for underground nuclear testing (Figure 1-1). Eighty-five underground nuclear tests were conducted at the PM CAUs between 1965 and 1992 (NNSA/NFO, 2015b). Underground nuclear tests deposit radioactive elements in the subsurface, resulting in groundwater contamination in the vicinity of the underground test locations. At the PM CAUs, the testing resulted in more than 2.68 × 10 7 curies (Ci) of radioactivity (decay-corrected to September 30, 2012) remaining underground (Finnegan et al., 2016). Of the 85 underground nuclear tests conducted at the PM CAUs, three were shallow tests detonated within 200 meters (m) of the surface and referred to as the “near-surface tests”; the remaining 82 were detonated deeper than 200 m below ground surface (bgs) and are referred to as the “deep underground tests” in this document.

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Assessing Effects of Climate Change on Legacy Waste at the Enewetak Atoll

The Republic of the Marshall Islands (RMI) is in the central Pacific Ocean ~4,500 km west of Hawaii. The Enewetak Atoll, located in the northwest part of the RMI, was the site for 43 nuclear weapon tests between 1948 and 1958. Fallout and deposition from the tests contaminated the island surfaces, lagoon waters and sediment, and nearby ocean waters at the atoll. In the 1970s, a cleanup effort collected radioactive waste and placed it in the Cactus Crater on Runit Island (also called the Runit Dome). In December 2021, Congress directed the U.S. Department of Energy to study the impacts of climate change on the Runit Dome nuclear waste disposal site. Pacific Northwest National Laboratory (PNNL) assembled a multidisciplinary team of climate scientists, ocean modelers, environmental scientists, and health physicists to assess the likely effects of remaining radionuclides at the Enewetak Atoll. PNNL’s approach focused on effects of tropical cyclones that were postulated to mobilize and transport contaminated lagoon sediments and result in human and biota exposure. PNNL’s study estimated (1) the radionuclide source term, (2) the effects of climate change on severe storms, (3) mobilization and transport of radionuclides, and (4) radiation dose to humans and biota. Radionuclides in the lagoon and/or ocean waters of the Enewetak Atoll were characterized by the U.S. Atomic Energy Commission (AEC) in 1972, Woods Hole Oceanographic Institution in 2015, and Lawrence Livermore National Laboratory in 2018. The RMI Nationwide Radiological Study was conducted in the early 1990s for radionuclides remaining in island soils. The 1972 AEC survey remains the most comprehensive source of radionuclide data on lagoon sediments. Climate change modeling at a regional scale in the central Pacific Ocean is limited. PNNL climate scientists simulated severe historical storms postulated to occur both in a recent climate (2015) and in the future (2090) using the Advanced Research Weather Research and Forecasting (WRF-ARW) model, employing a pseudo-global-warming technique. A postulated complete, future failure of the Runit Dome was also considered. PNNL developed a high-resolution regional ocean hydrodynamics model covering the entire RMI extended economic zone using the Finite Volume Coastal Ocean Model (FVCOM). The FVCOM model was run using global reanalysis data for current climate and WRF-ARW simulation for the future climate. PNNL also developed a radionuclide fate and transport model using the FVCOM Integrated Compartment Model (FVCOM-ICM) to simulate the current and future mobilization and transport of radionuclides sorbed to lagoon sediments and the exchange of radionuclides between the water and sediment. FVCOM-ICM-predicted radionuclide concentrations were then used to estimate radiation dose to humans and biota at all islands of the Enewetak Atoll. Under current climate conditions, annual radiation exposures for the southern islands including Enewetak (Fred) and Medren (Elmer) were below the current U.S. standards. Radiation doses were somewhat elevated starting at Runit Island northward and westward to Enjebi Island (Janet). The islands in the northwest quadrant, particularly Bokoluo (Alice) and Bokombako (Belle), remain relatively contaminated. The islands in the southwestern quadrant have low contamination. The highest contribution to radiation doses comes from consumption of locally grown foods. Two radionuclides, 90Sr and 137Cs, contributed the greatest fraction for most terrestrial foods. In current climate conditions, the storms temporarily increased radionuclide concentrations in the lagoon waters, increasing the radiation dose slightly. In future conditions, doses are expected to be smaller, primarily because of the radioactive decay of the shorter-lived radioisotopes of 90Sr and 137Cs. This could make all islands in the far northwest of the atoll – except Bokombako (Belle) and perhaps Bokoluo (Alice) – suitable for residency. For the f

Prasad, Rajiv↗

Using groundwater noble gas measurements to confirm paleorecharge hypotheses at Pahute Mesa, Nevada National Security Site, Nevada, USA

Pahute Mesa (Nevada, USA) was the site of 85 underground nuclear tests between 1965 and 1992 whose residual radio-chemical inventory poses a contaminant threat to local groundwater resources. To assess the fate and transport of these radionuclides in groundwater, several geochemical studies, including this one, have been conducted to understand long-term groundwater flow patterns at, and downgradient of, Pahute Mesa. Groundwater samples from the Pahute Mesa area at the Nevada National Security Site were analyzed for noble gases ( 3 He/ 4 He isotopic ratio and He, Ne, Kr, Ar and Xe concentrations) to infer groundwater recharge temperatures and provide additional evidence in support of groundwater flow patterns and the presence of late-pluvial Pleistocene groundwater. These data confirm recent findings (based on groundwater geochemistry and isotope compositions) that most recharge in the area occurred under temperature conditions much cooler than are found today, except near major drainages where ephemeral run of continues to recharge shallow groundwater. These noble gas data indicate that noble gas recharge temperatures and terrigenic He components have been reset where groundwater has flowed upward over barriers formed by caldera margins, or near the regional discharge area (Oasis Valley) where shallow groundwater has interacted with shallow soil gas. This evidence from groundwater noble gas measurements, in combination with other isotopic and geochemical studies, supports the current understanding of the unusual hydrogeology and recharge history of Pahute Mesa.

54 ENVIRONMENTAL SCIENCES↗

Synthesis of results for Brine Availability Test in Salt (BATS) DECOVALEX-2023 Task E

In the 2023 phase of the international collaborative DECOVALEX modeling project, Task E focused on understanding thermal, hydrological, and mechanical (THM) processes related to predicting brine migration in the excavation damaged zone around a heated excavation in salt. Salt is attractive as a disposal medium for radioactive waste because it is self-healing and is essentially impermeable and non-porous in the far field. Investigation of the short-term, near-field behavior is important for radioactive waste disposal because this early period strongly controls the amount of inflowing brine. Brine leads to corrosion of waste forms and waste packages, and possible dissolution of radionuclides with brine transport being a potential transport vector to the accessible environment.The Task was divided into steps. Step 0 included matching unheated brine inflow data from boreholes at the Waste Isolation Pilot Plant (WIPP) and matching temperature observations during a Brine Availability Test in Salt (BATS) heater test. Step 1 included validation of models against a thermo-poroelastic analytical solution, and two-phase flow around an excavation. Finally, Step 2 required all the individual components covered in steps 0 and 1 to come together to match observed brine inflow behavior during the same BATS heater test.There were a range of approaches from the teams, from mechanistic to prescriptive. Given the uncertainties in the problem, some teams used one- or two-dimensional models of the processes, while other teams included more geometrical complexity in three-dimensional models. Task E was a learning experience for the teams involved, and feedback from the modeling teams has led to changes in follow-on BATS experiments at WIPP. The primary Task E lessons learned were the impact of hydrologic initialization methods (wetting up vs. drying down), the difference between confined and unconfined thermal expansion, and the large changes in permeability associated with heating and cooling.

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Resilient design in nuclear energy: Critical lessons from a cross-disciplinary analysis of the Fukushima Dai-ichi nuclear accident

This paper presents a multidisciplinary analysis of the Fukushima Dai-ichi Nuclear Power Plant accident. Along with the latest observations and simulation studies, we synthesize the time-series and event progressions during the accident across multiple disciplines, including in-plant physics and engineering systems, operators’ actions, emergency responses, meteorology, radionuclide release and transport, land contamination, and health impacts. We identify three key factors that exacerbated the consequences of the accident: (1) the failure of Unit 2 containment venting, (2) the insufficient integration of radiation measurements and meteorology data in the evacuation strategy, and (3) the limited risk assessment and emergency preparedness. We conclude with new research and development directions to improve the resilience of nuclear energy systems and communities, including (1) meteorology-informed proactive venting, (2) machine learning-enabled adaptive evacuation zones, and (3) comprehensive risk-informed emergency planning while leveraging the experience from responses to other disasters.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Decovalex-2019 (Executive Summary)

The DECOVALEX Project is an on-going international research collaboration, established in 1992, to advance the understanding and modeling of coupled Thermal (T), Hydrological (H), Mechanical (M) and Chemical (C) processes in geological in geological systems. DECOVALEX was initially motivated by the recognition that prediction of these coupled effects is an essential part of the performance and safety assessment of geologic disposal systems for radioactive waste and spent nuclear fuel. Later it was realized that these processes also play a critical role in other subsurface engineering activities, such as subsurface CO 2 storage, enhanced geothermal systems, and unconventional oil and gas production through hydraulic fracturing. Research teams from many countries (e.g., Canada, China, Czech Republic, Finland, France, Germany, Japan, Republic of Korea, Spain, Sweden, Switzerland, Taiwan, United Kingdom, and the United States) various institutions have participated in the DECOVALEX Project over the years, providing a wide range of perspectives and solutions to these complex problems. These institutions represent radioactive waste management organizations, national research institutes, regulatory agencies, universities, as well as industry and consulting groups. The overall aim of DECOVALEX-2019 was to increase the understanding of various thermo-hydro-mechanical-chemical processes of importance for radionuclide release and transport from a repository to the biosphere and how they can be described and modelled using mathematical models. The scientific and technical objectives are: to increase the basic understanding of T-H-M-C coupled processes in fractured rocks (crystalline, sedimentary, argillaceous) and buffer materials; to investigate the predictive capabilities of different codes to field experiments and to perform verification of codes; to exchange experimental data, and improve the understanding of the constitutive behavior of crystalline and argillaceous rock masses and buffer materials; and to perform THMC calculations in a performance/safety assessment context.

58 GEOSCIENCES↗