The Influence of Thermal Gradients on the Long-Term Evolution of the Near-Field Environment of High-Level Nuclear Wastes Disposal

1997 ◽  
Vol 506 ◽  
Author(s):  
C. Poinssot ◽  
P. Toulhoat ◽  
B. Goffé

ABSTRACTThe initial stage of some HLW disposal systems will be characterised by a large thermal pulse in the near-field environment, due to the heat of the radioactivity decay. This will lead to the development of a transient spatial thermal gradient between the hot canister and the cold geological medium, which could significantly affect the composition and the elemental distribution within the near-field environment. A coupled experimental and modelling work is presented in order to determine the influence of a thermal gradient on water-rock interaction processes. First experiments with a simulated nuclear glass evidenced mass transfer processes leading to chemical differentiation in the solid phases between the hot and the cold end of the system. The relevance of these experimental results to the case of a HLW disposal is strongly supported by in-situ experiments at Stripa, in which a realistic EBS under thermal gradient developed exactly the same mass transfers.In order to understand the driving force of these processes, we tried to model simplified experiments by using a mixing cell geochemical model built upon the geochemical code EQ3/EQ6. The discrepancies between modelling and experiments indicate the existence of coupled processes involving irreversible precipitation.Finally, thermal gradients were applied in nuclear glass-clay interaction experiments to enhance elemental migrations. The main results are: (i) a re-crystallisation of the initial clay toward a more silicic one through incorporation of elements released by the glass, (ii) a strong influence of clay chemistry on the nuclear glass secondary phases.

1994 ◽  
Vol 353 ◽  
Author(s):  
Wunan Lin ◽  
D. G. Wilder ◽  
J. A. Blink ◽  
S. C. Blair ◽  
T. A. Buscheck ◽  
...  

AbstractThe radioactive decay heat from nuclear waste packages may, depending on the thermal load, create coupled thermal-mechanical-hydrological-chemical (TMHC) processes in the near-field environment of a repository. A group of tests on a large block (LBT) are planned to provide a timely opportunity to test and calibrate some of the TMHC model concepts. The LBT is advantageous for testing and verifying model concepts because the boundary conditions are controlled, and the block can be characterized before and after the experiment. A block of Topopah Spring tuff of about 3 × 3 × 4.5 m was sawed and isolated at Fran Ridge, Nevada Test Site. Small blocks of the rock adjacent to the large block were collected for laboratory testing of some individual thermal-mechanical, hydrological, and chemical processes. A constant load of about 4 MPa will be applied to the top and sides of the large block. The sides will be sealed with moisture and thermal barriers. The large block will be heated by heaters within and guard heaters on the sides so that a dry-out zone and a condensate zone will exist simultaneously. Temperature, moisture content, pore pressure, chemical composition, stress, and displacement will be measured throughout the block during the heating and cool-down phases. The results from the experiments on small blocks and the tests on the large block will provide a better understanding of some concepts of the coupled TMHC processes. The progress of the project is presented in this paper.


1986 ◽  
Vol 84 ◽  
Author(s):  
Mark M. Doxtader ◽  
Victor A. Maroni ◽  
James V. Beitz ◽  
Michael Heaven

The Basalt Waste Isolation Project (Rockwell Hanford Operations- BWIP) is investigating the feasibility of building a repository in the Columbia River Basalts for the permanent disposal of high-level nuclear waste. One aspect of this effort is to develop an understanding of the chemical behavior of radionuclides in the near-field environment of the waste container. Such information is needed to determine radionuclide release rates from the waste package and to make long-term projections of repository performance. To accomplish this task, ultrasensitive laser- based techniques, such as laser photoacoustic spectroscopy (LPAS) and laser induced fluorescence (LIF), are being developed as analytical methods for the trace-level detection and speciation of actinides in solutions typical of those encountered in groundwaters near the BWIP repository.


1997 ◽  
Vol 506 ◽  
Author(s):  
Peter C. Lichtner ◽  
Roberto T. Pabalan ◽  
Carl I. Steefel

ABSTRACTTo determine the potential effects of alkaline plume migration on the near-field environment of the proposed high-level radioactive waste geologic repository at Yucca Mountain, Nevada, calculations are conducted simulating interactions between cement and tuff with pure diffusive transport of solute species. The calculations used the reactive transport submodule GEM of the computer code MULTIFLO [6]. The results suggest that strong alteration of the tuff host rock and of cement in contact with the tuff could result from these interactions. Porosity reduction within the tuff could isolate the matrix from fracture pore water. The model calculations predict calcification of the cement as would be expected. In simulations involving counter-diffusive transport across the cement-tuff contact, calcification is more pronounced in a partially-saturated environment compared to a fully-saturated one.


1989 ◽  
Vol 176 ◽  
Author(s):  
A. Meike ◽  
W. E. Glassley

ABSTRACTA high temperature water vapor phase is expected to persist in the vicinity of high level radioactive waste packages for several hundreds of years. We have begun an investigation of the structural and chemical effects of water on cristobalite because of its abundance in the near field environment. A high voltage transmission electron microscope (HVEM) investigation of bulk synthesized α-cristobalite to be used in single phase dissolution and precipitation kinetics experiments revealed the presence β cristobalite, quartz and amorphous silica, in addition to α-cristobalite. Consequently, this apparent metastable persistence of β-cristobalite and amorphous silica during the synthesis of α-cristobalite was investigated using a heating stage and an environmental cell installed in the HVEM that allowed the introduction of either dry CO2 or a CO2 + H2O vapor. Preliminary electron diffraction evidence suggests that the presence of water vapor affected the α-β transition temperature. Water vapor may also be responsible for the development of an amorphous silica phase at the transition that may persist over an interval of several tens of degrees. The amorphous phase was not documented during the dry heating experiments.


Author(s):  
O. M. Katz

The swelling of irradiated UO2 has been attributed to the migration and agglomeration of fission gas bubbles in a thermal gradient. High temperatures and thermal gradients obtained by electron beam heating simulate reactor behavior and lead to the postulation of swelling mechanisms. Although electron microscopy studies have been reported on UO2, two experimental procedures have limited application of the results: irradiation was achieved either with a stream of inert gas ions without fission or at depletions less than 2 x 1020 fissions/cm3 (∼3/4 at % burnup). This study was not limited either of these conditions and reports on the bubble characteristics observed by transmission and fractographic electron microscopy in high density (96% theoretical) UO2 irradiated between 3.5 and 31.3 x 1020 fissions/cm3 at temperatures below l600°F. Preliminary results from replicas of the as-polished and etched surfaces of these samples were published.


Author(s):  
Christof Mast ◽  
Friederike Möller ◽  
Moritz Kreysing ◽  
Severin Schink ◽  
Benedikt Obermayer ◽  
...  

How does inanimate matter become transformed into animate matter? Living systems evolve by replication and selection at the molecular level and this chapter considers how to establish a synthetic, minimal system that can support molecular evolution and thus life. Molecular evolution cannot be explained by starting with high concentrations of activated chemicals that react toward their chemical equilibrium; persistent non-equilibria are required to maintain continuous reactivity and we especially consider thermal gradients as an early driving force for Darwinian molecular evolution. The temperature difference across water-filled compartments implements a laminar fluid convection with periodic temperature oscillations that allow for the melting and replication of DNA. Simultaneously, dissolved molecules are moved along the thermal gradient by an effect called thermophoresis. The combined result is an efficient molecule trap that exponentially favors long over short DNA and thus maintains complexity. Future experiments will reveal how thermal gradients could actively drive the Darwinian process of replication and selection.


2020 ◽  
Vol 45 (4) ◽  
pp. 319-332
Author(s):  
Xiaoyu Chen ◽  
Ruquan Liang ◽  
Yong Wang ◽  
Ziqi Xia ◽  
Lichun Wu ◽  
...  

AbstractThe effect of the temperature gradient on the Soret coefficient in n-pentane/n-decane (n-C5/n-C10) mixtures was investigated using non-equilibrium molecular dynamics (NEMD) with the heat exchange (eHEX) algorithm. n-Pentane/n-decane mixtures with three different compositions (0.25, 0.5, and 0.75 mole fractions, respectively) and the TraPPE-UA force field were used in computing the Soret coefficient ({S_{T}}) at 300 K and 1 atm. Added/removed heat quantities (ΔQ) of 0.002, 0.004, 0.006, 0.008, and 0.01 kcal/mol were employed in eHEX processes in order to study the effect of different thermal gradients on the Soret coefficient. Moreover, a phenomenological description was applied to discuss the mechanism of this effect. Present results show that the Soret coefficient values firstly fluctuate violently and then become increasingly stable with increasing ΔQ (especially in the mixture with a mole fraction of 0.75), which means that ΔQ has a smaller effect on the Soret coefficient when the temperature gradient is higher than a certain thermal gradient. Thus, a high temperature gradient is recommended for calculating the Soret coefficient under the conditions that a linear response and constant phase are ensured in the system. In addition, the simulated Soret coefficient obtained at the highest ΔQ within three different compositions is in great agreement with experimental data.


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