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At least 235 records · Page 13

Life Cycle Analysis and Life Cycle Costing for Municipal Solid Waste (MSW) Management and Materials Redeployment to Support ARPA-E’s Potential Program on Waste to Energy and Materials

Municipal solid waste infrastructure in the United States contains complex supply chains to transport, sort, and sequester waste. This project developed models to estimate the environmental and economic costs of waste infrastructure in the U.S. using data from several municipalities. Life cycle costing (LCC) models were developed for waste management relevant supply chain steps, including waste collection, sorting, landfilling, waste-to-energy, ash processing, and recycling. A waste-to-materials and energy (WTM&E) life cycle analysis (LCA) and LCC dashboard was developed in collaboration with Argonne National Laboratory (ANL) and an LCC tool was developed for additional analysis.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Preliminary Simulations of Commercial Drying Cycles Using the Advanced Drying Cycle Simulator

The purpose of this report is to document updates on the apparatus to simulate commercial vacuum drying procedures at the Nuclear Energy Work Complex at Sandia National Laboratories. Validation of the extent of water removal in a dry spent nuclear fuel storage system based on drying procedures used at nuclear power plants is needed to close existing technical gaps. Operational conditions leading to incomplete drying may have potential impacts on the fuel, cladding, and other components in the system during subsequent storage and disposal. A general lack of data suitable for model validation of commercial nuclear canister drying processes necessitates well-designed investigations of drying process efficacy and water retention. Scaled tests that incorporate relevant physics and well-controlled boundary conditions are essential to provide insight and guidance to the simulation of prototypic systems undergoing drying processes. This report documents fiscal year 2023 (FY23) updates on the Advanced Drying Cycle Simulator (ADCS). This apparatus was built to simulate commercial drying procedures and quantify the amount of residual water remaining in a pressurized water reactor (PWR) fuel assembly after drying. The ADCS was constructed with a prototypic 17×17 PWR fuel skeleton and waterproof heater rods to simulate decay heat. These waterproof heaters are the next generation design to heater rods developed and tested at Sandia National Laboratories in FY20. In FY23, a series of four simulated commercial drying tests was completed. This report presents the temperature and pressure histories of the drying tests as well as axial temperature profiles that can be compared to data from the Electric Power Research Institute (EPRI) High Burnup Demonstration TN-32B cask. Water content measurements and dew point calculations from a Hiden Analytical HPR-30 mass spectrometer are also presented in this report. Due to familiarization with this first-of-a-kind system, refinements to equipment calibration and test procedures have been identified to better match commercial drying cycles for future simulated tests. However, the presented data demonstrate the successful construction and operation of a viable research platform for quantifying residual water content closely approaching that expected in dry storage canisters during commercial drying procedures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Interactions between land use change and carbon cycle feedbacks: Land Use and Carbon Cycle Feedbacks

We explore the role of human land use and land cover change (LULCC) in modifying the terrestrial carbon budget in simulations forced by Representative Concentration Pathway 8.5, extended to year 2300 by using the Community Earth System Model, . Overall, conversion of land (e.g., from forest to croplands via deforestation) results in a model-estimated, cumulative carbon loss of 490 Pg C between 1850 and 2300, larger than the 230 Pg C loss of carbon caused by climate change over this same interval. The LULCC carbon loss is a combination of a direct loss at the time of conversion and an indirect loss from the reduction of potential terrestrial carbon sinks. Approximately 40% of the carbon loss associated with LULCC in the simulations arises from direct human modification of the land surface; the remaining 60% is an indirect consequence of the loss of potential natural carbon sinks. Because of the multicentury carbon cycle legacy of current land use decisions, a globally averaged amplification factor of 2.6 must be applied to 2015 land use carbon losses to adjust for indirect effects. This estimate is 30% higher when considering the carbon cycle evolution after 2100. Most of the terrestrial uptake of anthropogenic carbon in the model occurs from the influence of rising atmospheric CO 2 on photosynthesis in trees, and thus, model-projected carbon feedbacks are especially sensitive to deforestation.

58 GEOSCIENCES↗

Regime dependence of ice cloud heterogeneity – a convective life‐cycle effect?

Cloud condensate varies on scales smaller than those typically resolved by global weather and climate models. In order to accurately predict the radiative and microphysical process rates representative of the entire model grid box, the effect of the subgrid‐scale heterogeneity of cloud must be taken into account. In this study, observed ice water content retrieved from A‐Train satellite observations is used to explore how spatial ice condensate variability, characterized by the fractional standard deviation (FSD, the standard deviation divided by the mean), varies with cloud regime. FSD is generally lower for overcast cloud scenes, but an additional predictor based on convective activity is needed to capture the high FSD associated with more turbulent clouds and reproduce the observed latitudinal and height variations of FSD. Convective clouds that extend only a few kilometres above the freezing level are likely to be smaller at an earlier stage in their life cycle, and actively growing with a higher FSD. In contrast, more mature clouds reaching the tropopause are larger and generally have a lower variability and smaller FSD. To capture this life‐cycle effect, a new parametrization is tested which uses the ratio of a model's convectively detrained condensate to the existing cloud condensate mass as a proxy for the cloud's convective life stage to highlight areas with enhanced condensate variability. The parametrization is scale‐adaptive, situation‐dependent and captures seasonally varying global patterns and the zonal mean vertical structure of observed ice condensate variability well. Ground‐based observations obtained from five Atmospheric Radiation Measurement sites provide independent confirmation that the parametrization satisfactorily captures condensate variability in high‐altitude ice clouds.

Ahlgrimm, Maike↗

Fuel Cycle Considerations for Uranium, Plutonium and Minor Actinide Partitioning and Transmutation

This paper is written in memorial of the authors' past collaborations with Max Salvatores in the area of advanced nuclear fuel cycle evaluation. In this regard, a summary is provided of the results from two international studies led by Max Salvatores in which the authors participated: (1) the expert group on Homogeneous versus Heterogeneous Recycling of Transuranics in Fast Nuclear Reactors, and (2) the expert group on Potential Benefits and Impacts of Advanced Nuclear Fuel Cycles with Actinide Partitioning and Transmutation. Both of these studies presented the authors with the opportunity to contribute the results of past and ongoing research in the U.S., facilitating engagement and discussion on these subjects with researchers from other countries and organizations, resulting in the creation of broad international views on the relative benefits and challenges of transuranic recycle (NEA, 2012a; NEA, 2012b), a testament to the leadership and capabilities of Max Salvatores. Published by Elsevier Ltd.

Taiwo, Temitope↗

Heat Transfer Coefficients of Additively Manufactured Tubes with Internal Pin Fins for Supercritical Carbon Dioxide Cycle Recuperators

This paper describes the measurement of convective heat transfer coefficients and friction factors for sCO 2 flowing in additively manufactured tubes with internal pin fins at the US DOE’s National Energy Technology Laboratory in Morgantown, WV. The measurement procedures were validated by conducting benchmark tests with smooth stainless-steel tube and comparing the results with published correlations for Nusselt number (Nu) and friction factor. Over Reynolds numbers (ReD) ranging from 5 × 10 4 to 2.5 × 10 5 , measured Nu was within 5% of the Dittus-Boelter correlation and measured friction factors were within 5% of the McAdams correlation for smooth tube flow. The candidate pin fin patterned pipes were additively manufactured (AM) at the Oak Ridge National Laboratory. The pins were circular or elliptical in cross-section and were printed at a 30⁰ angle relative to the inner wall (to meet AM constraints). The pin arrangement was helical to promote enhanced heat transfer due to swirl flow. Pin length to diameter aspect ratio was 1.33, 2, and 8, while the pin diameter to tube diameter ratio was 0.188, 0.125, and 0.063. Tests were performed for ReD varying from 6.9 × 10 4 to 2.2 × 10 5 and at conditions equivalent to the low pressure (LP) outlet (8.69 MPa, 361 K) and the high pressure (HP) inlet (20.7 MPa, 350 K) of the low temperature recuperator (LTR) in an indirect sCO 2 cycle. The Wilson plot technique was utilized to measure the bulk heat transfer coefficients. For the best performing design (tube A, pin length to tube diameter ratio: 1.33, pin diameter to tube diameter ratio: 0.19), the local heat transfer coefficient increased by 136% relative to the Dittus-Boelter correlation at the LTR low pressure outlet and 194% at the LTR high pressure inlet. These correspond to a 282% and a 271% increase in the product of the heat transfer coefficient and surface area (adjusted for fin efficiency) product, respectively. Large pressure drops across the test articles were observed. For Tube Design A, the average friction factor, across the range of ReD considered, was significantly larger than the McAdams correlation at both the LTR LP outlet and the LTR HP inlet. A thermal performance factor was utilized to express the ratio of material required to build a finned heat exchanger relative to a finless heat exchanger with the same heat duty and pumping power. Tube Design A was estimated to decrease the required heat exchanger material by 13%.

Searle, Matthew↗

Can Mn–S redox cycling drive sedimentary dolomite formation? A hypothesis

The formation of dolomite in modern peritidal environments is linked to the degradation of buried microbial mats, with complexation of Ca and Mg by extracellular polymeric substances (EPSs) and alkalinity generation through organic carbon respiration facilitating the nucleation of dolomite precursors. In the past two decades, microbial sulfate reduction, methanogenesis, and methanotrophy have all been considered as potential drivers of the nucleation process, but it remains unclear why dolomite formation could not also occur in suboxic sediments where abundant alkalinity is produced by processes linked to Mn(IV) and/or Fe(III) reduction coupled with the diffusion and reoxidation of reduced sulfur species. Here we report the interstitial occurrence of spheroidal aggregates of nanometer-scale Ca-rich dolomite rhombohedra within suboxic sediments associated with remnant microbial mats that developed in the peritidal zone of the Archipelago Los Roques, Venezuela. Multiple analytical tools, including EPMA, ICP-MS, synchrotron-based XRF and XRD, and spatially resolved XANES microanalyses, show that the dolomite-cemented interval exhibits depleted bulk iron concentrations, but is interstitially enriched in Mn and elemental sulfur (S⁰). Manganese occurs in several oxidation states, indicating that the dolomite-cemented interval was the locus of complex biological redox transformations characterized by coupled Mn and S cycling. The tight correspondence between sedimentary Mn and MgCO₃ concentrations further hints at a direct role for Mn during dolomitization. While additional studies are required to confirm its relevance in natural settings, we propose a model by which coupled Mn–S redox cycling may promote alkalinity generation and thus dolomite formation in manner similar to, or even more efficiently, than bacterial sulfate reduction alone.

58 GEOSCIENCES↗

Improved cycling behavior of ZEBRA battery operated at intermediate temperature of 175°C

Operation of sodium-nickel chloride battery at temperatures lower than 200°C reduces cell degradation and improves the cyclability. One of the main technical issues in terms of operating this battery at intermediate temperatures such as 175°C is the poor wettability of molten sodium on β”-alumina solid electrolyte (BASE) causing reduced active area and limited charging . In order to overcome the problem related to poor wettability of Na melt on BASE at 175°C, Pt grid was applied on the anode side of BASE using a screen printing technique. Deeper charging and improved cycling behavior was observed on the cells with metalized BASEs due to extended active area.

intermediate temperature↗

Effects of cycling temperatures on the voltage fade phenomenon in 0.5Li 2 MnO 3 ·0.5LiNi 0.375 Mn 0.375 Co 0.25 O 2 cathodes

The rate of voltage fade in 0.5Li2MnO3•0.5LiNi0.375Mn0.375Co0.25O2 cathodes was measured in half-cells in a temperature range of 25 to 55°C. On the basis of the dependence of the values of the open-circuit potential with cycle count and temperature, the voltage fade phenomenon seems to consist of two chemical processes: one that can be described using a parabolic rate law and another that uses a linear-with-time law. As the cycling temperature increased, the relative contributions of the two processes changed. On the basis of the overall rate versus temperature data, we believe the two processes may be in competition with one another.

kinetics↗

Cobalt-Group 13 Complexes Catalyze CO 2 Hydrogenation via a Co(-I)/Co(I) Redox Cycle

The Co(-I) dihydrogen complexes, [(η 2 -H 2 )CoML]-, where ML is the group 13 metalloligand, N(o-(NCH 2 PiPr 2 )C 6 H 4 ) 3 M, and M is Al, Ga, or In, were previously reported ( J. Am. Chem. Soc. 2017, 139, 6570-6573). In this work, the related Co(-I) end-on dinitrogen adducts, [(N 2 )CoML]-, were isolated and investigated as precatalysts for CO 2 hydrogenation. The Co–Ga catalyst was highly active, achieving 19,200 formate turnovers with an initial turnover frequency of 27,000 h –1 under 34 atm of 1:1 CO 2 /H 2 and using Verkade’s proazaphosphatrane as a base at ambient temperature. The Co–Al catalyst was moderately active, while the Co–In complex was inactive. Hence, tuning the group 13 ion greatly influences the catalytic activity at the Co site. To elucidate the role of the group 13 support, experimental and theoretical mechanistic studies of the Co–Ga and Co–Al catalysts were conducted. The Co(-I) H 2 species are potent hydride donors with estimated thermodynamic hydricities (ΔG° H– ) of 32.0(1) and 37.4(1) kcal/mol in CH 3 CN for M = Al and Ga, respectively. By acting as masked Co(I) dihydrides, the Co(-I) H 2 species operate via an unusual Co(-I)/Co(I) redox cycle. After hydride transfer to CO 2 , the resulting intermediate is the Co(I) hydride complex, HCoML, which was independently synthesized and structurally characterized for M = Al and Ga. The Gibbs free energy for H 2 binding, ΔG° bind (1 atm), to generate (η 2 -H 2 )HCoML was slightly more favorable for HCoGaL (-4.2(1) kcal/mol) than for HCoAlL (-2.7(1) kcal/mol). In the subsequent step, the deprotonation reaction to regenerate the initial catalyst was much more favorable for (η 2 -H 2 )HCoGaL (pK a of 31.4, CH 3 CN) than for (η 2 -H 2 )HCoAlL (pK a of 34.3). Finally, the straightforward substitution of Al with Ga perturbs the energy profile of the catalytic reaction (|ΔΔG° H– | = 5.4 kcal/mol, |ΔΔG° bind | = 1.5 kcal/mol, and |ΔΔG° K a | = 4.0 kcal/mol) and thus provides a thermodynamic rationale for the higher catalytic efficiency of Co–Ga over Co–Al.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Biostimulation induces syntrophic interactions that impact C, S and N cycling in a sediment microbial community

Stimulation of subsurface microorganisms to induce reductive immobilization of metals is a promising approach for bioremediation, yet the overall microbial community response is typically poorly understood. Here we used community proteogenomics to test the hypothesis that excess input of acetate activates syntrophic interactions among autotrophs and heterotrophs. A flow-through sediment column was incubated in a groundwater well of an acetate-amended aquifer. Genomic sequences from the community recovered during microbial sulfate reduction were used to econstruct, de novo, near-complete genomes for Desulfobacter (Deltaproteobacteria) and relatives of Sulfurovum and Sulfurimonas (Epsilonproteobacteria), and Bacteroidetes. Partial genomes were obtained for Clostridiales (Firmicutes) and Desulfuromonadales-like Deltaproteobacteria. The majority of proteins identified by mass spectrometry corresponded to Desulfobacter-like species, and demonstrate the role of this organism in sulfate reduction (Dsr and APS), nitrogen-fixation (Nif) and acetate oxidation to CO2 during amendment. Results suggest less abundant Desulfuromonadales and Bacteroidetes also actively contributed to CO2 production via the TCA cycle. Proteomic data indicate that sulfide was partially re-oxidized by Epsilonproteobacteria through nitrate-dependent sulfide oxidation (using Nap, Nir, Nos, SQR and Sox), with CO2 fixed using the reverse TCA cycle. Modeling shows that this reaction was thermodynamically possible, and kinetically favorable relative to acetate-dependent denitrification. We conclude that high-levels of carbon amendment aimed to stimulate anaerobic heterotrophy led to carbon fixation in co-dependent chemoautotrophs. These results have implications for understanding complex ecosystem behavior, and show that high levels of organic carbon supplementation can expand the range of microbial functionalities accessible for ecosystem manipulation.

metagenomics/proteomics/subsurface/sediment/syntro↗