Microscopic and spectroscopic bioassociation study of uranium(VI) with an archaeal Halobacterium isolate

The safe disposal of high-level radioactive waste in a deep geological repository is a huge social and technical challenge. So far, one of the less considered factors needed for a long-term risk assessment, is the impact of microorganisms occurring in the different host rocks. Even under the harsh conditions of salt formations different bacterial and archaeal species were found, e. g. Halobacterium sp. GP5 1–1, which has been isolated from a German rock salt sample. The interactions of this archaeon with uranium(VI), one of the radionuclides of major concern for the long-term storage of high-level radioactive waste, were investigated. Different spectroscopic techniques, as well as microscopy, were used to examine the occurring mechanisms on a molecular level leading to a more profound process understanding. Batch experiments with different uranium(VI) concentrations showed that the interaction is not only a simple, but a more complex combination of different processes. With the help of in situ attenuated total reflection Fourier-transform infrared spectroscopy the association of uranium(VI) onto carboxylate groups was verified. In addition, time-resolved laser-induced luminescence spectroscopy revealed the formation of phosphate and carboxylate species within the cell pellets as a function of the uranium(VI) concentration and incubation time. The association behavior differs from another very closely related halophilic archaeon, especially with regard to uranium(VI) concentrations. This clearly demonstrates the importance of studying the interactions of different, at first sight very similar, microorganisms with uranium(VI). This work provides new insights into the microbe-uranium(VI) interactions at highly saline conditions relevant to the long-term storage of radioactive waste in rock salt.

Investigation of Re(VII) diffusion in Tamusu clayrock core by through-diffusion method

Tamusu area is the primary pre-selection site of clayrock disposal repository for high-level radioactive waste (HLW) in China. However, the research on the migration behavior of nuclides in Tamusu clayrock is still in its infancy. For the first time in laboratory, the diffusion behavior of Re(VII) in Tamusu clayrock core was studied by means of through-diffusion method. The effects of pH, ionic strength and humic acid on the diffusion behavior of Re(VII) in clayrock were studied. The effective diffusion coefficient, apparent diffusion coefficient and rock capacity factor value were obtained. All the experimental conditions of Re(VII) diffusion in Tamusu clayrock are compared with other geological samples under the same conditions in literature data. The diffusion mechanism of radionuclide in Tamusu clay is discussed, which can provide experimental data for site selection and safety assessment of high-level radioactive waste repository in China. The experimental results showed an effective application and reference for the countries disposed HLW in mudrocks or clayrocks, such as France, Belgium etc. in Europe. Moreover, this research can provide the original data support for the metallogenic regularity and prospecting prognosis of rare element rhenium in different geological environments.

Section 14 StandAG – Identification of siting regions and associated challenges

With the publication of the subarea interim report on sub-regions on 28 September 2020, the Federal Company for Radioactive Waste Disposal (BGE), as the implementer of the German site selection procedure, has completed the first step of phase I in due time. The second step of phase I is the identification of siting regions for surface exploration. In the following step 2 of phase I, the determination of siting regions for surface exploration will be carried out based on the interim results of the first step of phase I in accordance with section 14 of the regulating law (StandAG). A central component of this second step of phase I is the representative preliminary safety assessments pursuant to section 27 StandAG, the ordinances on “Safety Requirements” (EndlSiAnfV) and “Preliminary Safety Assessments” (EndlSiUntV), which are carried out for each of the sub-regions. Based on the results of the preliminary safety assessments and the renewed application of the geoscientific weighting criteria (section 24 StandAG), siting regions will be identified that have the potential to become the site with the best possible safety for a repository for high-level radioactive waste. During the second step of phase I, the planning scientific consideration criteria (section 25 StandAG) can be applied for the first time. The path to the siting regions for surface exploration can be accompanied by various challenges related to geoscientific, methodological and also societal questions. For example, the application of the representative preliminary safety assessments may be more challenging in larger subareas compared to smaller ones as subsurface properties are likely to be more variable. In this context, areas with little data coverage for example, and the treatment of these areas in the procedure may pose another challenge. Therefore, sound methodological concepts must be developed for performing the representative preliminary safety assessments as well as for applying the geoscientific weighting criteria. Furthermore, the German site selection procedure defines special requirements (section 1 StandAG): the implementation of the participatory, science-based, transparent, self-questioning and learning procedure poses challenges to all stakeholders of the procedure on the way to the best possible disposal of high-level radioactive waste.

Microscopic and spectroscopic investigations of uranium(VI) reduction by <i>Desulfosporosinus hippei</i> DSM 8344

Clay formations are potential host rocks for the long-term storage of high-level radioactive waste in a deep geological repository. Bentonites are supposed to serve as backfill material, not only for a final disposal site in clay formations but also in crystalline rock. For a long-term safety assessment, various aspects must be taken into account. Besides geological, geochemical and geophysical considerations, naturally occurring microorganisms also play a crucial part in the environment of such a repository. In the event of a worst-case scenario when water enters the disposal site, they can interact with the radionuclides and change for example the chemical speciation or the oxidation state (Lloyd et al., 2002). Desulfosporosinus spp. are an important representative of anaerobic, sulfate-reducing microorganisms, which are present in clay formations as well as in bentonites. Various studies have shown that they play a major role in the microbial communities of these surroundings (Bagnoud et al., 2016; Matschiavelli et al., 2019). A closely related microorganism to the isolated species is Desulfosporosinus hippei DSM 8344, which was originally found in permafrost soil (Vatsurina et al., 2008). This bacterium was used to investigate its interactions with uranium(VI) especially regarding the reduction to the less mobile uranium(IV). Time-dependent reduction experiments in artificial Opalinus Clay pore water (Wersin et al., 2011) (100 µM uranium(VI), pH 5.5) showed the removal of about 80 % of the uranium(VI) from the supernatants within 48 h. Corresponding UV/Vis measurements of the dissolved cell pellets exhibited an increasing proportion of uranium(IV) in the cell-bound uranium. Calculations with the inclusion of extinction coefficients led to a ratio of 39 % uranium(IV) after 1 week. Therefore, a combined sorption-reduction process is a possible interaction mechanism. Time-resolved laser-induced luminescence spectroscopy verified the presence of two uranium(VI) species in the supernatant. A comparison with reference spectra led to an assignment to a uranyl(VI) lactate and a uranyl(VI) carbonate complex. The species distribution showed a decrease of the proportion of the lactate species with time, whereas the proportion of the carbonate species remained almost constant. Uranium aggregates are formed on the cell surface during the process, as determined by transmission electron microscopy (TEM). Furthermore, uranium occurs inside and outside the cells as well as vesicles containing uranium. These findings help to close existing gaps in a comprehensive safeguard concept for a repository for high-level radioactive waste in clay rock. Moreover, this study provides new insights into the interactions of sulfate-reducing microorganisms with uranium(VI).

Identification and evaluation of processes for joint disposal of high level radioactive waste and low to intermediate level radioactive waste

The on-going research project „Identification and evaluation of processes that can arise by disposing of both high level radioactive waste (HAW) and low to intermediate level radioactive waste (LAW/MAW) at the same site“ (GemEnd, FKZ 4719F10401), commissioned by the Federal Office for the Safety of Nuclear Waste Management (BASE), is concerned with the question which thermal, hydraulic, mechanical, chemical and biological (THMCB) processes could be of importance for the long-term safety of the geological repository for high level radioactive waste. The focus of the project is on mutual influences between the HAW and LAW/MAW repositories, which should be constructed separately according to the Safety Regulations (Federal Ministry for the Environment, Nature Conservation and Nuclear Safety, BMU, 2020). A second point of emphasis is on processes that could result from the disposal of small amounts of LAW/MAW within the HAW repository. The analyses carried out for each of the potential host rocks clay rock, rock salt and crystalline rock as well as for a combination of clay rock above crystalline rock at a generic site are divided into a qualitative and a quantitative part. As for the qualitative analyses, all potentially relevant processes are identified and evaluated as to whether they are negligible or principally relevant for the exemplary repository configurations considered and according to the current state of knowledge. With regard to the quantitative analyses, the possible extent of potentially safety-relevant processes is illustrated by means of coupled numerical simulations. Of special interest are the effects of particularly sensitive model approaches and/or parameters and notably of the distances between the HAW and LAW/MAW repositories in the different exemplary repository configurations considered. From the results of the quantitative and qualitative analyses, knowledge gaps will be identified and the possibility of their reduction by research and development activities will be discussed. Furthermore, aspects of the transferability of the results to the German site selection procedure will be illuminated. At the interdisciplinary research symposium safeND selected preliminary results of both the qualitative and quantitative analyses will be presented.

On the temperature in a final disposal site for high-level radioactive waste

The Site Selection Act stipulates a precautionary temperature limit of 100 ∘C on the outer surface of the containers with high-level radioactive waste (HLRW) in the final disposal site. This precautionary temperature limit should be applied in preliminary safety analyses provided that the maximum physically possible temperatures in the respective host rocks have not yet been determined due to pending research. Increasing temperatures in the deep geological underground, caused by the heat generation of the HLRW, can trigger thermal, hydraulic, mechanical, chemical and biological processes (THMCB) in the respective host rocks of a final disposal site and thus endanger safety. Furthermore, high temperatures may hamper the feasibility to retrieve and recover HLRW from a final disposal site. Such processes are described in detail in databases for features, events and processes (FEP) databases. Single components or barriers of a final disposal facility may require specific design temperatures for the preservation of their features once a concept for long-term safety of a final disposal site is established; however, the interactions of all relevant processes of a concept for a final disposal site must be considered when a specific temperature limit for the outer surface of the containers is derived. This temperature limit may vary for particular safety and final disposal concepts in the host rock: salt, clay and crystalline rock. The conclusion is that temperature limits regarding the outer surface of the containers should be derived specifically for each safety and disposal concept and should be supported by a solid safety analysis. Temperature limits without reference to specific safety concepts or the particular design of the final disposal site likely narrow down the possibilities for optimisation and could adversely affect the site selection process in finding the best suitable site.