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At least 1,171 records · Page 65

Dry cask radiation shielding validation and estimation of cask surface dose rate with MAVRIC during long-term storage

The dry storage cask became a semi-permanent solution for spent nuclear fuel since no permanent solution has been finalized over the past three decades. Considering the difficulty of deep geological repository projects in many aspects, prolonging the service life of dry casks longer than a few decades has become an option for spent nuclear fuel storage. It must be ensured that dry cask safety objectives, including radiation shielding, criticality safety, structure health, decay heat removal, and containment be fulfilled during the prolonged service life. This paper presents numerical modeling results of the radiation dose rate distribution on a TN-32 cask surface aged up to 300 years. The numerical modeling method was validated with measurement data, and the difference between the calculated results and measurement data in the total dose rate is 7%. The detailed radiation distribution variations over cask surfaces along the axial and radial directions for 300 years of storage were obtained, and their azimuthal angular dependence was established. The maximum total dose rate over the cask surfaces is less than 10 mrem/hour (9.258 ± 0.212 mrem/hour) after 40 years, and this outcome fulfills all dose rate requirements from 10 CFR 71.47(b). After 300 years of storage, the average total dose rates on the side surface and top surface are 0.150 ± 0.007mremmrem/hour and 0.057 ± 0.003mremmrem/hour, respectively, while the maxima are 0.601 ± 0.014 mrem/hour and 0.112 ± 0.006 mrem/hour, respectively. The variations in the fuel gamma ray, structure gamma ray, neutron and secondary gamma-ray contributions to the total dose rate are presented and analyzed in this work. The neutron and gamma-ray dose rate contributions by energy group are presented and analyzed at the cask top, mid-plane, and bottom at the selected storage times.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

What is the long-term demand for liquid hydrocarbon fuels and feedstocks?

Liquid hydrocarbons made from crude oil serve many functions: (1) a dense, easy-to-store, easy-to-transport energy source, (2) a method for daily-to-seasonal energy storage, (3) a chemical feedstock, (4) a chemical reducing agent and (5) a method to enhance high-temperature heat transfer in many furnaces and industrial processes. Liquid hydrocarbons can be produced and used without increasing atmospheric carbon dioxide levels if made from non-fossil feedstocks such as carbon dioxide or biomass. Understanding future liquid hydrocarbon demand is the starting point in assessing the viability of such options. Our assessment is that U.S. demand for liquid hydrocarbons is unlikely to go below the equivalent of 10 million barrels per day of crude oil but could be as high as 20 million barrels per day. The costs to replace liquid hydrocarbons increases rapidly at lower liquid hydrocarbon consumption rates. Hydrocarbon biofuels from cellulosic feedstocks can meet such demands if produced with large external inputs of heat and hydrogen. Options based on more limited feedstocks (starches, plant oils, sugars, etc.) can’t meet such demands.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Assessment of the impacts of renewable energy variability in long-term decarbonization strategies

To meet the nationally determined contributions proposed by the countries that signed the Paris Agreement, investments must be made in renewable generation technologies such as solar and wind. However, due to their high variability, these technologies pose challenges in terms of meeting demand or generating excess electricity. For this reason, energy system models are designed to capture this variability by considering flexibility technologies. Nevertheless, it is important to note that some energy system models lack integration with other sectors. Therefore, integrated assessment models have been employed to evaluate mitigation strategies, as they endogenously consider the linkages between energy and non-energy sectors. In addition, due to their complexity, these models do not account for the variability of renewable resources. Hence, this research aims to address this issue. Here, this work represents the first attempt to evaluate how the introduction of hourly resolution affects the outcomes of integrated assessment models, specifically focusing on the Global Change Analysis Model (GCAM). We employ a soft-linking approach between the GCAM and the Highway to Renewable Energy Systems model (H2RES, an hourly level energy system model) to accomplish this. The proposed approach is tested using Chile’s Nationally Determined Contributions under different hydrological profiles in the power sector. The results show that it is possible to use the capacity obtained from the Global Change Analysis Model and implement it on an hourly scale. However, the feasibility of implementation depends on high levels of flexibility technologies, such as battery energy storage. When given the choice of investments in renewable sources and flexible technologies, the optimal dispatch of the H2RES model show small differences than those obtained by GCAM-Chile. H2RES differs from GCAM-Chile in approximately 5% for wind and 3% for solar electricity generation in the year 2050. However, feasible integration of significant renewable sources is obtained with relatively high Critical Excess Electricity Production levels, reaching 20% in 2050. This excess electricity is attributed to the necessity for flexible technologies to manage the intermittency of renewables sources when hourly profiles of such sources are considered.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Long-term carbon emission reduction potential of building retrofits with dynamically changing electricity emission factors

Buildings account for approximately 36% of the United States' total carbon emissions and building retrofits have great potential to reduce carbon emissions. Current research adopts a constant electricity emission factor although it changes over time due to the increase of renewable energy generation. Here, to accurately predict emission reduction potential of building retrofits, this study develops a novel method by using dynamically changing electricity emission factors. Using medium office buildings as an example, we predicted emission reduction of eight building retrofit measures from 2020 to 2050 in five locations in the U.S. with distinct climates and renewable adoption rates. To evaluate emission reduction potential sensitivity to the compositions of electricity generation, five scenarios for renewable energy adoptions are investigated. The results reveal several new phenomena on emission reduction potential of building retrofits for medium offices in the U.S.: (1) it decreases from 2026 to 2050; (2) it has the same trend with coal usage; and (3) it reaches the maximum under the high renewable cost scenario. Based on the results, it is recommended that building retrofits should focus on 1) improving lighting and equipment efficiency; 2) locations with higher coal usage rate, and 3) buildings under the high renewable cost scenario. The new method can also be used for predicting emission reduction potential of the building sector in the U.S. by applying to other building types and regions.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Impact of anion-exchange membrane degradation on long-term CO 2 electrolysis to ethylene

Electrochemical CO 2 reduction (eCO2R) to ethylene offers a unique opportunity to diversify domestic supply chains for chemical manufacturing. Large-scale deployment of eCO2R to ethylene reactors is currently limited by low energy efficiencies and poor durability. Herein, we demonstrate >100 h of continuous electrolysis at an industrially relevant current density of 200 mA cm −2 in a 25 cm 2 geometric area zero-gap reactor with a full-cell voltage <3.1 V and ethylene Faradaic efficiency >30%. Incorporating expanded polytetrafluoroethylene (PTFE)-supported electrodes into zero-gap reactors allows for durable electrode catalysts that are resistant to flooding, and this enables wider ranges of operating parameters not typically accessible in CO 2 electrolysis. Finally, we identify membrane degradation, evidenced by a loss of membrane ion-exchange capacity, as the leading cause of performance loss over 144 h of electrolysis.

Energy - Conversion↗

On the long-term migration of uranyl in bentonite barrier for high-level radioactive waste repositories: The effect of different host rocks

Repositories for high level radioactive waste hosted in argillite or granite with bentonite backfill are the two disposal concepts that been extensively studied. A general perception is that granite has very low sorption capacity and therefore is disadvantageous in retarding the migration of radionuclides in comparison with argillite. However, when there is bentonite backfill, does the sorption capacity of granite really matter for the migration of radionuclides? How different host rocks would affect the migration of U(VI) through the bentonite backfill of an engineered barrier system (EBS), and which properties of the host rocks cause those differences in migration, given that migration of radionuclides is a critical measure in assessing the performance of a repository? Here we present two coupled thermal, hydrological, and chemical models for the transport of U(VI), each with an identical setup except for the type of host rock (argillite vs granite rock). Comparisons between our models show that the different host rocks exert their influence on migration of U(VI) via regulating the chemical conditions in the bentonite, which affect the concentration of U(VI) at the source and the adsorption of U(VI) in the bentonite. The key chemical conditions are pH, Ca + , and HCO 3 - concentration in pore-water, which are strongly affected by soluble carbonate minerals. Our models also show the occurrence of illitization (dissolution of smectite and precipitation of illite) in the bentonite, which affects the migration of U(VI) through changing pH and the quantity of adsorbents. Although generalization of current model results for granite and argillite should be done carefully, the simulations highlight the importance of pore-water chemistry in host rock, as well as bentonite-host rock interactions, when assessing the performance of a repository. In comparison to properties such as thermal conductivity, permeability, and adsorption capacity, properties that have been studied intensively, the pore-water chemistry of host rocks deserve equal or even more attention because of its strong influence on radionuclide migration.

58 GEOSCIENCES↗

Influence of ethylenediaminetetraacetic acid on the long-term oxidation state distribution of plutonium

Here, spectrophotometry was used to study the effect of EDTA on plutonium oxidation state distribution as a function of time, pH, and ligand-to-metal ratio (L/M) under anoxic conditions. Novel Pu(V)-EDTA absorption bands were identified at 571, 993, 1105, and 1150 nm with molar absorption coefficients of 15 ± 1, 6 ± 1, 10 ± 1, and 10 ± 1 cm –1 M –1 , respectively. Pu(V)-EDTA spectral changes occurred at L/M < 1, indicating only Pu V O 2 (EDTA) 3- formed with logK = 3.6 ± 0.3. Time-resolved experiments showed EDTA drastically increased the Pu(V/VI) reduction rate, which we propose is driven by amine lone-pair electron donation and the oxidative decarboxylation of EDTA. Oxidation of Pu(III)-EDTA to Pu(IV)-EDTA occurred on a slower time scale (110–237 days) than previously reported (<15 min) and is hypothesized to be radiolysis driven. Pu(V/VI)-EDTA and Pu(III)-EDTA both approached Pu(IV)-EDTA stabilization over time, yet Pu(V/VI)-EDTA solubility data was ≥ 1.0 log 10 units higher than predicted by Pu(IV)-EDTA solubility models, indicating that current thermodynamic models are incomplete. Ultimately, the data show EDTA preferentially stabilizes Pu(IV) over time regardless of initial oxidation state, but Pu(V)-EDTA can persist under environmentally-relevant conditions, emphasizing the need to continue investigating redox reactions, speciation, and behavior of these complexes to support the transuranic waste disposal and surface remediation/containment efforts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗