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At least 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
NASA NTRS2003

Process for Nitrogen Oxide Waste Conversion to Fertilizer

The present invention describes a process for converting vapor streams from sources containing at least one nitrogen-containing oxidizing agent therein to a liquid fertilizer composition comprising the steps of: a) directing a vapor stream containing at least one nitrogen-containing oxidizing agent to a first contact zone; b) contacting said vapor stream with water to form nitrogen oxide(s) from said at least one nitrogen-containing oxidizing agent; c) directing said acid(s) as a second stream to a second contact zone; d) exposing said second stream to hydrogen peroxide which is present within said second contact zone in a relative amount of at least 0.1% by weight of said second stream within said second contact zone to convert at least some of any nitrogen oxide species or ions other than in the nitrate form present within said second stream to nitrate ion; e) sampling said stream within said second contact zone to determine the relative amount of hydrogen peroxide within said second contact zone; f) adding hydrogen peroxide to said second contact zone when a level of hydrogen peroxide less than 0.1 % by weight in said second stream is determined by said sampling; g) adding a solution comprising potassium hydroxide to said second stream to maintain a pH between 6.0 and 11.0 within said second stream within said second contact zone to form a solution of potassium nitrate; and h) removing said solution of potassium nitrate from said second contact zone.

Lueck, Dale E.↗
NASA NTRS2007

Dust Modeling with GEOS-Chem: Evidence for Acidic Uptake on Dust Surfaces during INTEX-B

We use measurements of aerosol ion composition and size made from the DC8 aircraft during the 2006 INTEX-B airborne campaign to identify mineral dust signatures, and look for evidence for interaction of dust with acidic components. Coating of dust with sulfate or nitrate favors the role of dust particles as cloud condensation nucleii, can promote further uptake of SO2 and N2O5, can impact NOx/HNO3 partitioning, and can shift sulfate or nitrate towards larger sizes, affecting atmospheric lifetimes for both aerosol and gas components. Mineral dust had a pervasive presence on flights made during the Northern Pacific deployment of the INTEX-B mission. We use scatter plots of ion mixing ratios with Na+ and Ca(2+) to distinguish sea salt and mineral components of the aerosol distribution, respectively. Positive correlations of non-sea-salt sulfate and nitrate with calcium indicate that the dusty air stream is associated with polluted air masses. Sulfate-ammonium scatter plots indicate sulfate to be primarily in the form of (NH4)2SO4. A positive correlation between Ca(2+) and NO-, but little evidence of NH4NO3, suggests that NO3- may be associated with mineral dust surfaces. 3-d model simulations conducted with the GEOS-Chem chemical transport model indicate that transpacific transport from East Asia was principally responsible for the dust observed from the aircraft over the Pacific. We compare the aerosol component relationships in the model with those observed. Uptake of sulfate and nitrate on the dust is not yet represented in the model.

Fairlie, T. Duncan↗
NASA NTRS2006

Role of Climate Change in Global Predictions of Future Tropospheric Ozone and Aerosols

A unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies general circulation model II is applied to simulate an equilibrium CO2-forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5-20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2-driven climate change alone is predicted to reduce the global O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate-sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate-induced changes in burdens and different climatological conditions; with full gas-aerosol coupling and accounting for ozone and direct radiative forcings by the O2, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, -0.72, -1.0, +1.26, and -0.56 W m(exp -2), respectively, using present-day climate and year 2100 emissions, while they are predicted to be +0.76, -0.72, 0.74, +0.97, and -0.58 W m(exp -2), respectively, with year 2100 climate and emissions.

Liao, Hong↗
NASA NTRSDate not supplied

Consequences of Insufficient Production of Temporary NOx Reservoirs on Ozone Production in Models During KORUS-AQ

The advent of geostationary satellites, starting with GEMS over South Korea, offer the potential for additional insight into urban air quality. In preparation for these satellites, the joint NIER-NASA KORUS-AQ field campaign in 2016 obtained a large dataset for understanding local air quality and the contribution of local emissions to ozone and PM2.5 pollution. Models partitioned NOx primarily into inorganic nitrate (HNO3 + nitrate aerosol) while observations suggest that acyl peroxy nitrates (PNs) should be an important sink. Models tended to produce ozone too efficiently, which may be due to insufficient alkyl/multifunctional nitrate (ANs) production. Models are unable to simulate the transport of NOx away from the urban center and its impact on ozone production downwind.

Katherine R Travis↗
NASA NTRS2022

Measurement report: Closure Analysis of Aerosol–cloud Composition in Tropical Maritime Warm Convection

Cloud droplet chemical composition is a key observable property that can aid understanding of how aerosols and clouds interact. As part of the Clouds, Aerosols and Monsoon Processes – Philippines Experiment (CAMP2Ex), three case studies were analyzed involving collocated airborne sampling of relevant clear and cloudy air masses associated with maritime warm convection. Two of the cases represented a polluted marine background, with signatures of transported East Asian regional pollution, aged over water for several days, while the third case comprised a major smoke transport event from Kalimantan fires. Sea salt was a dominant component of cloud droplet composition, in spite of fine particulate enhancement from regional anthropogenic sources. Furthermore, the proportion of sea salt was enhanced relative to sulfate in rainwater and may indicate both a propensity for sea salt to aid warm rain production and an increased collection efficiency of large sea salt particles by rain in subsaturated environments. Amongst cases, as precipitation became more significant, so too did the variability in the sea salt to (non-sea salt) sulfate ratio. Across cases, nitrate and ammonium were fractionally greater in cloud water than fine-mode aerosol particles; however, a strong covariability in cloud water nitrate and sea salt was suggestive of prior uptake of nitrate on large salt particles. A mass-based closure analysis of non-sea salt sulfate compared the cloud water air-equivalent mass concentration to the concentration of aerosol particles serving as cloud condensation nuclei for droplet activation. While sulfate found in cloud was generally constrained by the sub-cloud aerosol concentration, there was significant intra-cloud variability that was attributed to entrainment – causing evaporation of sulfate-containing droplets –and losses due to precipitation. In addition, precipitation tended to promote mesoscale variability in the sub-cloud aerosol through a combination of removal, convective downdrafts, and dynamically driven convergence. Physical mechanisms exerted such strong control over the cloud water compositional budget that it was not possible to isolate any signature of chemical production/loss using in-cloud observations. The cloud-free environment surrounding the non-precipitating smoke case indicated sulfate enhancement compared to convective mixing quantified by a stable gas tracer; however, this was not observed in the cloud water (either through use of ratios or the mass closure), perhaps implying that the warm convective cloud timescale was too short for chemical production to be a leading-order budgetary term and because precursors had already been predominantly exhausted. Closure of other species was truncated by incomplete characterization of coarse aerosol (e.g., it was found that only 10 %–50% of sea salt mass found in cloud was captured during clear-air sampling) and unmeasured gasphase abundances affecting closure of semi-volatile aerosol species (e.g., ammonium, nitrate and organic) and soluble volatile organic compound contributions to total organic carbon in cloud water.

Ewan Crosbie↗
NASA NTRSDate not supplied

A Simulated High CO 2 Spaceflight Environment Increases Plant Preference for Ammonium as a Nitrogen Source

Long-duration exploration missions will require a sustainable supply of food to support human crews. The spaceflight environment contains high concentrations of CO 2 due to release by astronauts that cannot be completely scrubbed. It is therefore crucial to understand plant responses to elevated CO 2 (eCO 2 ) environments. Nitrogen (N) is crucial for plant survival, though the effects of eCO 2 on plant N uptake remain poorly understood. Shoot nitrate reduction may be reduced at eCO 2 , due to reduced reductant availability for nitrate reduction due to reduced photorespiration and increased carbon fixation. Relative growth rate may be reduced at eCO 2 when N is provided only as nitrate and can be unaffected when N is supplied as ammonium, suggesting eCO 2 may drive increased plant ‘preference’ for ammonium. However, changes in N preference in response to eCO 2 have, to our knowledge, not yet been studied. In this study, novel stable isotope approaches were used in conjunction with hydroponics and isotope ratio mass spectrometry to determine the effect of space station-like eCO 2 (3000 ppm) on preference for ammonium or nitrate in several lettuce varieties previously grown in space, when both N forms are provided equally. All varieties displayed significant ammonium preference irrespective of CO 2 concentration, however the extent of this preference varied. Increased ammonium preference was observed for all varieties at eCO 2 compared to ambient CO 2 (410 ppm), driven by increases in nitrogen uptake which plants disproportionately took up as ammonium. These results suggest that future nutrient formulations should favor ammonium as a major N source for space crop production. Moreover, increased ammonium preference may play a role in future plant-based bioregenerative life support systems with higher ammonium concentrations due to waste recycling. Additionally, this research furthers our understanding of plant responses to future high CO 2 climates, allowing the development of future-proof crops to maintain food security.

space crop production↗
DOE OSTI2022

Rapid pyrolysis to form super ionic conducting lithium garnets

A method of preparing a lithium-ion conducting garnet via low-temperature solid-state synthesis is disclosed. The lithium-ion conducting garnet comprises a substantially phase pure aluminum-doped cubic lithium lanthanum zirconate (Li 7 La 3 Zr 2 O 14 ). The method includes preparing nanoparticles comprising lanthanum zirconate (La 2 Zr 2 O 7 -np) via pyrolysis-mediated reaction of lanthanum nitrate (La(NO 3 ) 3 ) and zirconium nitrate (Zr(NO 3 ) 4 ). The method also includes pyrolyzing a solid-state mixture comprising the La 2 Zr 2 O 7 -np, lithium nitrate (LiNO 3 ), and aluminum nitrate (Al(NO 3 ) 3 ) to give the Li 7 La 3 Zr 2 O 14 and thereby prepare the lithium-ion conducting garnet. A lithium-ion conducting garnet prepared via the method is also disclosed.

Daemen, Luc L.↗
DOE OSTI2025

Generation and Study of Am(IV) by Temperature-Controlled Electron Pulse Radiolysis

Used nuclear fuel (UNF) separation techniques that strive to separate radiotoxic americium (Am) from trivalent lanthanide fission products through oxidation state control have increased research efforts surrounding Am(V) and Am(VI). However, equivalent knowledge of the tetravalent state, Am(IV), has remained elusive, particularly in conditions more representative of UNF reprocessing, i.e., in concentrated nitric acid (HNO3). With this in mind, we have used electron pulse radiolysis to study the radiation-induced redox reaction of Am(III) with the oxidizing nitrate radical (NO3?) in 6 M HNO3: Am(III) + NO3? ? Am(IV) + NO3? . These experiments enabled us to observe the growth and decay of Am(IV) in a concentrated acidic solution for the first time. The transient Am(IV) species was found to have a lifetime of ~16 µs?sufficiently long-lived to play a critical mechanistic role in UNF reprocessing systems. Additionally, we performed the first-ever temperature-dependent kinetics study of an actinide element, elucidating unprecedented Arrhenius and Eyring activation parameters for the reaction of Am(III) with NO3?. This new knowledge provides much-needed molecular-level insights into the radiation-induced behavior of Am.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Carbon sequestration and nitrogen and phosphorus accumulation in a freshwater, estuarine marsh: Effects of microtopography and nutrient loads

Wetlands are widely recognized as nutrient sinks for their ability to remove nutrients in runoff and retain them in soils. This is a valuable service, especially in agricultural watersheds, making nutrient removal one of the main goals in many wetland creation and restoration projects. However, incorporating nutrient management considerations requires site-level assessments, the scale at which wetland creation and restoration occur. Here we studied how carbon (C) sequestration, and nitrogen (N) and phosphorus (P) accumulation vary at different microtopographic levels and locations within a freshwater, estuarine marsh on the coast of Lake Erie. We further explored links between C sequestration, and N and P accumulation in recent years, and orthophosphate ($PO_{4}^{3-}$), ammonium ($NH_{4}^{+}$), and nitrate ($NO_{3}^{-}$) concentrations and loads. The rates of C sequestration and N accumulation were relatively lower at spots of intermediate depth and locations closer to the wetland’s main channel. P accumulation was highest at deep spots but did not differ among locations based on distance from the channel. Empirical models showed that nitrate load is the most important variable explaining the variability in C, N, and P sequestration/accumulation (r2 = 0.57, 0.61, and 0.32, respectively) and that the relationship between inorganic nutrient loads and accumulation was negative. Our findings suggest that including microtopographic relief features in wetland creation and design, especially deeper spots, is critical to enhancing wetland ecosystems’ C, N, and P sinking capacity. Also, that upstream nitrate management should be a priority to increase benefits from C sequestration and long-term N and P accumulation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Structural features of early fuel cycle taggant incorporation for intentional nuclear forensics

To develop strategies for incorporating transition metal taggants (Fe, Cr, and Ni) into oxide fuels and to understand how these taggant candidates persist through early fuel cycle processes, synthetic procedures are modified from established production routes to yield intentionally tagged early fuel cycle intermediates including uranyl nitrate hexahydrate (UNH, UO 2 (NO 3 ) 2 ·6H 2 O), uranyl peroxide tetrahydrate (studtite, UO 2 O 2 ·4H 2 O), and uranyl peroxide dihydrate (metastudtite, UO 2 O 2 ·2H 2 O). First, Fe, Cr, and Ni nitrate solutions are introduced to an aqueous solution of UNH followed by precipitation to produce tagged UNH. Then, studtite is precipitated from UNH followed by dehydration to metastudtite. Structural influences of taggant incorporation within all synthesized phases are investigated using powder X-ray diffraction (PXRD) and Raman spectroscopy to provide insight into crystallographic modifications resulting from the addition of tags to these early fuel cycle materials and elucidate the chemical form of taggants introduced at these stages. The possibility of segregation of taggant species into discrete phases within U matrices was examined using scanning electron microscopy with energy dispersive X-ray spectroscopy. Taggant concentrations in solid-phase materials were determined using inductively coupled plasma-optical emission spectroscopy. Observations from Raman spectroscopy and PXRD indicate that introducing transition metal tags during uranyl nitrate precipitation results in potential impurity phase segregation in UNH, but transition metal incorporation is suggested by results for tagged uranyl peroxide materials. Further, results from this study will inform strategies for optimizing taggant incorporation in UO 2 .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Effect of Electrolyte Ions on Iridium Oxide-Based Water Oxidation Catalysis

The oxygen evolution reaction often limits the efficiency of renewable fuel syntheses due to its sluggish reaction kinetics. Of the factors that have been studied to improve this important reaction is how the choice of the electrolyte may alter the reaction kinetics. Despite its importance, sys-tematic studies of this effect have been relatively rare. Herein, we report an effort toward correcting this deficiency by investigating the effect of nitrate on water oxidation catalyzed by IrO x . The results show that nitrate can suppress the reaction, resulting in a decrease of the rate and an increase in the Tafel slope. The effect was found to be consistent with a microkinetic model incorporating competitive adsorption between reac-tion intermediates and nitrate, suggesting that the reaction mechanism was unaffected by anion identity. Moreover, this blocking effect exhibited dependence on the cations, following a trend Li + ≈ Na + ≈ K + > Cs + > TEA + . The results are expected to find broad applications in electrocatalysis.

Tafel slope analysis↗
DOE OSTI2024

Genomic and environmental controls on Castellaniella biogeography in an anthropogenically disturbed subsurface

Castellaniella species have been isolated from a variety of mixed-waste environments including the nitrate and multiple metal-contaminated subsurface at the Oak Ridge Reservation (ORR). Previous studies examining microbial community composition and nitrate removal at ORR during biostimulation efforts reported increased abundances of members of the Castellaniella genus concurrent with increased denitrification rates. Thus, we asked how genomic and abiotic factors control the Castellaniella biogeography at the site to understand how these factors may influence nitrate transformation in an anthropogenically impacted setting. We report the isolation and characterization of several Castellaniella strains from the ORR subsurface. Five of these isolates match at 100% identity (at the 16S rRNA gene V4 region) to two Castellaniella amplicon sequence variants (ASVs), ASV1 and ASV2, that have persisted in the ORR subsurface for at least 2 decades. However, ASV2 has consistently higher relative abundance in samples taken from the site and was also the dominant blooming denitrifier population during a prior biostimulation effort. We found that the ASV2 representative strain has greater resistance to mixed metal stress than the ASV1 representative strains. We attribute this resistance, in part, to the large number of unique heavy metal resistance genes identified on a genomic island in the ASV2 representative genome. Additionally, we suggest that the relatively lower fitness of ASV1 may be connected to the loss of the nitrous oxide reductase (nos) operon (and associated nitrous oxide reductase activity) due to the insertion at this genomic locus of a mobile genetic element carrying copper resistance genes. This study demonstrates the value of integrating genomic, environmental, and phenotypic data to characterize the biogeography of key microorganisms in contaminated sites.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Re-Designing the CSP Thermal Energy Storage System to Enable Higher-Temperature Performance at Reduced Cost (Final Technical Report)

Current commercial concentrating solar power (CSP) plants distinguish themselves from ordinary photovoltaic (PV) power plants by storing enough collected energy to enable generation for several hours after the sun goes down. CSP plants store this energy in the sensible heat of nitrate salts in large metallic storage tanks. Stainless-steel AISI 347H (SS347H) is needed for the hot tank operating at about 565 degrees C whereas carbon steel is sufficient for the cold-tank materials. Two-tank nitrate-salt thermal energy storage (TES) is presently in use in several trough-based CSP plants in Europe and in the U.S., operating up to about 390 degrees C. Three commercially operating tower-based CSP plants - Gemasolar in Spain, Crescent Dunes in Nevada, and Noor III in Morocco - use the same approach, storing nitrate salts at temperatures up to 580 degrees C. SS347H is many times more expensive than carbon steel and constitutes a significant cost element in today's CSP plants. Hence, CSP developers need to close the cost gap with PV-based solar plants by making cost reductions in every system of the plant. Redesigning the TES tanks is one opportunity for cost reduction.

14 SOLAR ENERGY↗
DOE OSTI2021

Mono- and Dinitro-BN-Naphthalenes: Formation and Characterization

Mono- and dinitro-BN-naphthalenes, i.e., 1-nitro-, 3-nitro-, 1,6-dinitro-, 3,6-dinitro-, and 1,8-dinitro-BNN, were generated in the nitration of 9,10-BN-naphthalene (BNN), a boron–nitrogen (BN) bond-embedded naphthalene, with AcONO 2 and NO 2 BF 4 in acetonitrile. The nitrated products were isolated and characterized by NMR, GC-MS, IR, and X-ray single crystallography. The effects of the nitration on the electron density and aromaticity of BNN were evaluated by B-11 NMR analysis and HOMA calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

BSEC Air Quality: Stationary Aerosol Composition and Mass Concentration at Baltimore

Data is 10-min average mass composition and mass concentration from the TOF-ACSM-X. TOF-ACSM-X reports fine (less than 2.5 um diameter) non-refractory aerosol, including organic aerosol, sulfate, nitrate, ammonium, and non-refractory chloride. Also reported is the elemental ratios determined for organic aerosol (O/C, H/C, and organic matter to organic carbon ratio, OM/OC). Finally, ion ratios of key ions used for identifying sources, ammonium balance, and fractional contribution of organic nitrate aerosol to total aerosol nitrate has been included.

aerosol↗
NASA NTRS2016

Directional and Spectral Irradiance in Ocean Models: Effects on Simulated Global Phytoplankton, Nutrients, and Primary Production

The importance of including directional and spectral light in simulations of ocean radiative transfer was investigated using a coupled biogeochemical-circulation-radiative model of the global oceans. The effort focused on phytoplankton abundances, nutrient concentrations and vertically-integrated net primary production. The importance was approached by sequentially removing directional (i.e., direct vs. diffuse) and spectral irradiance and comparing results of the above variables to a fully directionally and spectrally-resolved model. In each case the total irradiance was kept constant; it was only the pathways and spectral nature that were changed. Assuming all irradiance was diffuse had negligible effect on global ocean primary production. Global nitrate and total chlorophyll concentrations declined by about 20% each. The largest changes occurred in the tropics and sub-tropics rather than the high latitudes, where most of the irradiance is already diffuse. Disregarding spectral irradiance had effects that depended upon the choice of attenuation wavelength. The wavelength closest to the spectrally-resolved model, 500 nm, produced lower nitrate (19%) and chlorophyll (8%) and higher primary production (2%) than the spectral model. Phytoplankton relative abundances were very sensitive to the choice of non-spectral wavelength transmittance. The combined effects of neglecting both directional and spectral irradiance exacerbated the differences, despite using attenuation at 500 nm. Global nitrate decreased 33% and chlorophyll decreased 24%. Changes in phytoplankton community structure were considerable, representing a change from chlorophytes to cyanobacteria and coccolithophores. This suggested a shift in community function, from light-limitation to nutrient limitation: lower demands for nutrients from cyanobacteria and coccolithophores favored them over the more nutrient-demanding chlorophytes. Although diatoms have the highest nutrient demands in the model, their relative abundances were generally unaffected because they only prosper in nutrient-rich regions, such as the high latitudes and upwelling regions, which showed the fewest effects from the changes in radiative simulations. The results showed that including directional and spectral irradiance when simulating the ocean light field can be important for ocean biology, but the magnitude varies with variables and regions. The quantitative results are intended to assist ocean modelers when considering improved irradiance representations relative to other processes or variables associated with the issues of interest.

Phytoplankton↗
NASA NTRS2024

Evaluation of CMIP6 Model Simulations of PM 2.5 and its Components Over China

Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM 2.5 ) as major climate forcers. Yet the model performance for PM 2.5 components remains little evaluated due in part to a lack of observational data. Here, we evaluate near-surface concentrations of PM 2.5 and its five main components over China as simulated by 14 CMIP6 models, including organic carbon (OC; available in 14 models), black carbon (BC; 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM 2.5 components. Seven models output total PM 2.5 concentrations, and they all underestimate the observed total PM 2.5 over eastern China, with GFDL-ESM4 (−1.5 %) and MPI-ESM-1-2-HAM (−1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM 2.5 from the available component output, underestimate the total PM 2.5 concentrations partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by −71.2 % to −37.8 % across the 14 models) and the smallest for BC (−47.9 % to −12.1 %). The multi-model mean (MMM) reproduces the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.74) fairly well, yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM 2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing.

CMIP6↗
DOE OSTI2020

Developing and Implementing New Waste Chemistry Controls for Hanford's Double-Shell Tanks - 20041

Waste chemistry controls for the Hanford double-shell tanks (DSTs) were established in the 1980's in response to tank failures caused by stress corrosion cracking (SCC) at the Savannah River Site (SRS). The controls were established based on a combination of SRS chemistry limits and corrosion testing results. Conditions in the Hanford DSTs have changed over time, with the temperature in the majority of the DSTs dropping below 50 deg. C. Testing indicated that the original chemistry control specification and SCC testing performed in 2010 did not protect against pitting corrosion mechanisms - what is believed to have caused the failure of tank 241-AY-102. New waste chemistry controls are necessary to protect the DSTs from both SCC and pitting corrosion. Savannah River National Laboratory (SRNL), with input from the Tank Integrity Expert Panel (TIEP) Corrosion Subgroup (CSG), performed a statistically based investigation of nitrate and halide ion induced pitting corrosion. The investigation was intended to develop a comprehensive waste chemistry envelope that minimizes the risk of both SCC and pitting caused by halide and nitrate ions. The waste chemistry envelope needed to be robust enough to address future waste retrieval and process changes which could significantly change the waste composition of the DSTs. The experimental design allowed the statistically significant ions and their effect on pitting corrosion to be determined. SRNL developed the 'pitting factor' which is an empirical relationship between the statistically significant inhibitive species (hydroxide, and nitrite), and pitting inducing species (nitrate, chloride, and fluoride). The coefficients are weighted factors that show the degree of influence the species have on the propensity for pitting. New waste chemistry control limits were recommended by SRNL, and concurred with by the TIEP CSG, that incorporated the pitting factor along with other limits. The controls developed to reduce the risk of pitting corrosion were evaluated to determine if they also protected against SCC. Hundreds of test results were reviewed and compared against the proposed limits. With the exception of one test result, instances where cracking was observed corresponded to chemistry that was outside of the proposed limits - indicating that the chemistry controls developed for pitting also adequately addressed SCC concerns. Existing tank composition estimates were evaluated against the new chemistry controls - three current tank chemistries are suspect, and may not meet the new chemistry control requirements. These included the interstitial liquid (liquid associated with solids) of DSTs 241-AN-102, 241-AN-106, 241-AN-107, and 241-AY-101. Measures are ongoing to evaluate the tanks with the suspect chemistry. These include varying combinations of: performing additional evaluations (history of use, modeling); DST specific laboratory testing; and, pursuing core samples of the DSTs. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗