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Evaporation of Cu, Sn, and S from Fe-C-Cu-Sn-S Liquid Alloys in the Temperature Range from 1513 K to 1873 K (1240 °C to 1600 °C)

Evaporation of Cu or Sn from liquid iron alloys containing C and S was experimentally investigated. The initial C concentration, [pct C] 0 , in the liquid alloy was varied from zero to C saturation, and the evaporation temperature was varied from 1513 K to 1773 K (1240 °C to 1500 °C). Along with the report by one of the present authors, the evaporation mechanism of Cu and Sn from liquid Fe-C-S alloy is proposed, after a modification from the previous mechanism. It was proposed that Cu and Sn evaporate as Cu(g) and Sn(g) and also evaporate as CuS(g) and SnS(g), which are more volatile species. Therefore, availability of S in the alloy affects the overall evaporation rate of Cu and Sn. At the same time, C in the alloy also forms volatile carbosulfides CS(g) and CS 2 (g), thereby competing with Cu and Sn. Moreover, C increases the activity coefficients of Cu, Sn, and S. This increases the thermodynamic driving force for the formation of CuS(g) and SnS(g). Therefore, increasing [pct C] partly accelerates the evaporation rate of Cu and Sn by increasing the activity coefficient but partly decelerates the evaporation rate by lowering the available S content. S partly accelerates the evaporation rate by increasing the available S for the sulfide gas species but partly decelerates the evaporation rate due to the surface poisoning effect. Increasing the reaction temperature increases the overall evaporation rate. All these facts were taken into account in order to develop an evaporation rate model. This model was extended from the present authors’ previous one by taking into account (1) CS(g), S(g), and CS{ 2 (g) (therefore, the following species were considered as dominant evaporating species: Cu(g), CuS(g), Sn(g), SnS(g), S(g), CS(g), and CS 2 (g)); (2) the effect of C and temperature on the activity coefficients of Cu, Sn, and S; (3) the effect of C and temperature on the density of the liquid alloy; and (4) the effect of temperature on the S adsorption coefficient. This revised evaporation model was used in order to explain the experimental data, and it showed good agreement. In particular, it was found that the temperature showed a significant effect on the evaporation rate, and the effect of temperature and C content on the activity coefficients of Cu, Sn, and S also significantly affected the evaporation rate. The chemical reaction rate constant of the individual evaporation reaction (k i } R ) and residual rate constant (k i r ) could be obtained as a function of temperature. The activation energy of each evaporation reaction was derived and discussed. The evaporation rate model can be applied in order to predict the content of Cu and Sn remaining in liquid iron under various conditions of temperature and [pct C].

36 MATERIALS SCIENCE↗

Optimization of Delignified Wood Rods for Interfacial Solar Evaporation

Interfacial solar evaporation using three-dimensional evaporator materials has shown promise to achieve high evaporation rates exceeding the photothermal limit for water treatment and resource recovery processes. However, challenges remain in optimizing the material geometry to balance the vertical capillary uptake of water and the rate of evaporation to achieve both stable and high evaporation rates. Delignified wood can serve as a highly porous and hydrophilic substrate material to achieve high evaporation rates. In this work, we designed a suspended biochar-coated delignified wood rod evaporator and investigated the influence of its geometric parameters on its evaporation performance. The height of the evaporator exposed to air for evaporation was observed to be an important parameter in governing the evaporation rate, as shorter evaporators limited the available surface area for evaporation, but taller evaporators could not achieve sufficient rates of capillary uptake to maintain stable evaporation rates over 24 h under 1-sun illumination (1 kW m –2 ). In conclusion, the exposed height of the evaporator was optimized to achieve an average hourly evaporation rate of 3.05 ± 0.23 kg m –2 h –1 , which could be maintained in saline solutions containing up to 5 wt % NaCl.

Coating materials↗

Modeling the Effect of Evaporative Flux and Colloidal Aggregation on Crud Deposition

During the last few years lot of research has been conducted to investigate and predict the Crud deposition in PWRs. One of the common findings of various experimental and computational studies is that thickness or amount of crud deposits is directly related to evaporative flux maps. Evaporation driven deposition profile on the surfaces takes different forms, i.e. from ring to disk shapes during initial stages and in the form of porous to impervious continuous layers covering the hot fuel surface at the later stages. The amount and thickness of these deposits although are directly related to evaporative flux, the relationship is much complex and can be dependent upon several other factors. A popular problem relating evaporative flux to particulate deposition has been well studied in the form of drying of sessile colloidal drops. It was proposed that, this phenomenon is due to a geometrical constraint: the free surface, constrained by a pinned contact line squeezes the fluid outwards to compensate for evaporative losses and thereby transporting particles to the contact line. Later on a quantitative relationship between evaporative flux and deposition rate was proposed and validated by the same group, which showed power-law relationship. Deposition studies conducted with controlled concentration of particles with subcooled nucleate boiling also showed a power-law relationship rather than a simpler linear relationship whereas physics of evaporation would tend to concentrate particles at linear rate. In a typical subcooled nucleate boiling system, bubble growth and departure time is of the order 1-2 ms, measured experimentally. Diffusion time constant for dilute spherical metallic colloids such as crud particulates, generally present as particulate in process piping, range from 0.0025-2.5 sec in water for a size range 0.1-1.0 μm. Colloidal behavioral characteristics during the growth of bubbles can be computed with escape time constant at collision, which is dependent on effective Hamaker constant. For minimum effective Hamaker constant of Hematite is -2.5 kT and diffusion time constant τ = 0.0025 sec, escape time constant is computed as Kramer rule, τexp[A/kT] magnitude is 0.03 sec or 30 ms. This clearly indicates that evaporation will cause particles to come together and they cannot escape at a fast enough rate which would lead them to form agglomerates. Therefore both effects of evaporative flux in conjunction with the agglomeration kinetics must be considered for modeling the crud deposition if the evaporative flux is known. In this paper, we propose a phenomenological model of colloidal transport and aggregation with evaporative flux. The dynamic of particles interactions while drying of sessile colloidal drops is developed by coupling general transport equation with Smoluchowshki Coagulation equation. Crud deposition on the nuclear fuel has been a serious problem with severe consequences in nuclear power plants. In several studies it has been consistently reported that crud deposition is directly related to evaporative flux on the nuclear fuel surfaces. However, it has not been established how to quantify the deposition rates of crud type particulates if the evaporative flux is known. This complex multiphysics problem is similar to coffee-ring effect, where the governing physics is understood more clearly. In this work, a simplified geometry is used to model the effects of evaporative flux acting at a boundary on the colloidal concentration. The effect of this condition on change in concentration is shown numerically. Further, agglomeration is suspected to play a significant role in high evaporative flux such as bubble nucleation. The coagulation kinetics is modeled using uniform particle distribution and the effective total concentration of colloids including original particles and agglomerates is studied. Once this model is validated with a simple separate effect experiments, it can be integrated to large scale PWR models of evaluating evaporative flux and chemistry models developed by Electrical Power Research Institute (EPRI). (authors)

42 ENGINEERING↗

Laboratory studies of 2H evaporator scale dissolution in dilute nitric acid

The rate of 2H evaporator scale solids dissolution in dilute nitric acid has been experimentally evaluated under laboratory conditions in the SRNL shielded cells. The 2H scale sample used for the dissolution study came from the bottom of the evaporator cone section and the wall section of the evaporator cone. The accumulation rate of aluminum and silicon, assumed to be the two principal elemental constituents of the 2H evaporator scale aluminosilicate mineral, were monitored in solution. Aluminum and silicon concentration changes, with heating time at a constant oven temperature of 90 deg C, were used to ascertain the extent of dissolution of the 2H evaporator scale mineral. The 2H evaporator scale solids, assumed to be composed of mostly aluminosilicate mineral, readily dissolves in 1.5 and 1.25 M dilute nitric acid solutions yielding principal elemental components of aluminum and silicon in solution. The 2H scale dissolution rate constant, based on aluminum accumulation in 1.5 and 1.25 M dilute nitric acid solution are, respectively, 9.21E-04 ± 6.39E-04 min{sup -1} and 1.07E-03 ± 7.51E-05 min{sup -1}. Silicon accumulation rate in solution does track the aluminum accumulation profile during the first few minutes of scale dissolution. It however diverges towards the end of the scale dissolution. This divergence therefore means the aluminum-to-silicon ratio in the first phase of the scale dissolution (non-steady state conditions) is different from the ratio towards the end of the scale dissolution. Possible causes of this change in silicon accumulation in solution as the scale dissolution progresses may include silicon precipitation from solution or the 2H evaporator scale is a heterogeneous mixture of aluminosilicate minerals with several impurities. The average half-life for the decomposition of the 2H evaporator scale mineral in 1.5 M nitric acid is 12.5 hours, while the half-life for the decomposition of the 2H evaporator scale in 1.25 M nitric acid is 10.8 hours. Based on averaging the two half-lives from the 2H scale acid dissolution in 1.25 and 1.5 M nitric acid solutions, a reasonable half-live for the dissolution of 2H scales in dilute nitric acid is 11.7 ± 1.3 hours. The plant operational time for chemically cleaning (soaking) the 2H evaporator with dilute nitric acid is 32 hours. It therefore may require about 3 half-lives or less to completely dissolve most of the scales in the Evaporator pot which come into contact with the dilute nitric acid solution. On a mass basis, the Al-to-Si ratio for the scale dissolution in 1.5 M nitric acid averaged 1.30 ± 0.20 and averaged 1.18 ± 0.10 for the 2H scale dissolution in 1.25 M nitric acid. These aluminum-to-silicon ratios are in fairly good agreement with ratios from previous studies. Therefore, there is still more aluminum in the 2H evaporator scales than silicon which implies that there are no significant changes in scale properties which will exclude nitric acid as a viable protic solvent for aluminosilicate scale buildup dissolution from the 2H evaporator. Overall, the monitoring of the scale decomposition reaction in 1.25 and 1.5 M nitric acid may be better ascertained through the determination of aluminum concentration in solution than monitoring silicon in solution. Silicon solution chemistry may lead to partial precipitating of silicon with time as the scale and acid solution is heated.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Interfacial Solar Evaporation by a 3D Graphene Oxide Stalk for Highly Concentrated Brine Treatment

In this study, we demonstrate a 3-dimensional graphene oxide (3D GO) stalk that operates near the capillary wicking limit to achieve an evaporation flux of 34.7 kg m -2 h -1 under 1 sun conditions (1 kW/m 2 ). This flux represents nearly a 100 times enhancement over a conventional solar evaporation pond. Interfacial solar evaporation traditionally uses 2D evaporators to vaporize water using sunlight, but their low evaporative water flux limits their practical applicability for desalination. Some recent studies using 3D evaporators demonstrate potential for more efficient water transfer, but the flux improvement has been marginal because of a low evaporation area index (EAI), which is defined as the ratio of the total evaporative surface area to the projected ground area. By using a 3D GO stalk with an ultrahigh EAI of 70, we achieved nearly a 20-fold enhancement over a 2D GO evaporator. The 3D GO stalk also exhibited additional advantages including omnidirectional sunlight utilization, a high evaporation flux under dark conditions from more efficient utilization of ambient heating, a dramatic increase of the evaporation rate by introducing wind, and scaling resistance in evaporating brines with a salt content of up to 17.5 wt %. This performance makes the 3D GO stalk well suited for the development of a low-cost, reduced footprint technology for zero liquid discharge in brine management applications.

3D evaporator↗

Atmospheric humidity deficits tell us how soil moisture deficits down-regulate ecosystem evaporation

Knowing how actual evaporation is down-regulated from potential evaporation during periods with soil moisture deficits is one of the greatest challenges towards computing evaporation everywhere on a regular basis. We propose the hypothesis that vegetated landscapes transmit information on soil moisture deficits through its down-regulation of evaporation, which in turn affects the humidification and growth of the planetary boundary layer. To test this hypothesis, here, we examined how the evaporative fraction, defined as the ratio between actual and potential evaporation, corresponds with the soil moisture stress index, defined as the relative humidity with a power law dependence on vapor pressure deficit times a parameter, β. We tested the parameterized soil moisture stress index with direct eddy covariance measurements of actual evaporation and computations of potential evaporation based on meteorological conditions, averaged on monthly time steps. The analysis was conducted on a dataset obtained from 144 FLUXNET sites. These sites spanned much of the world's climates and biomes and contained over 5900 months of observations. Observations of the evaporative fraction fit the model of the soil moisture stress index best for semi-arid and arid ecosystems, and least for the humid and wet ecosystems. Consequently, a significant relationship between measurements of the evaporative fraction and soil moisture stress index held for about one-half of the population of sites. Under this condition, the median value of the parameter, β, was 1.41. To investigate the mechanism of this empirical soil moisture stress index, we diagnosed it with a coupled evaporation-planetary boundary layer model. The soil moisture stress index is strongly related to surface resistance, as defined by inverting Penman-Monteith equation. Consequently, this index provides an independent estimate of surface resistance based on easy to measure mean monthly weather conditions like relative humidity and temperature. Thereby, this soil moisture stress index has potential to be applied to weather, climate and biogeochemical models and the interpretation of satellite derived evaporation products, like the one provided by the ECOSTRESS mission.

54 ENVIRONMENTAL SCIENCES↗

Trends and meteorological drivers of extreme daily reservoir evaporation events in the western United States

Extreme daily evaporation from reservoir surfaces can lead to significant short-term water losses, affecting water quality, water supply, and reservoir operation strategies. Historical trends in daily reservoir evaporation events have eluded the scientific and operational communities, largely due to a lack of long-term, consistent data record. This study quantifies trends in extreme daily reservoir evaporation events at 165 major reservoirs located in the western U.S. Here, we use the place-based energy balance and aerodynamic Daily Lake Evaporation Model (DLEM) driven by multiple meteorological data products (RTMA, gridMET, Daymet) to estimate daily evaporation rates at these reservoirs from 1981 to 2022. The results—while are based on different meteorological forcing datasets—consistently indicate that the California, Lower Colorado, and Rio Grande hydrologic regions are more prone to higher daily evaporation extremes. Compared to the rest of western U.S, these three regions also experience a more pronounced increasing trend in the annual maximum daily evaporation rate, at about 0.3 mm day -1 decade -1 during 1981-2022. The results show that heat and dryness are the main drivers to the increasing trend of extreme evaporation, while extreme wind speed is the primary contributor to exceptionally high daily evaporation events across all regions. This phenomenon is particularly prominent in the arid Lower Colorado region, but less significant in the cold and humid Pacific Northwest region. We also find that the correlation between extreme wind speed and extreme evaporation degrades as the time scale increases from daily, to monthly and seasonal. Our findings have strong implications for the pattern and distribution of extreme evaporation events at the western U.S. reservoirs, and illustrate how various drivers influence extreme evaporation across different time scales.

13 HYDRO ENERGY↗

Loss and Isotopic Fractionation of Alkali Elements during Diffusion-Limited Evaporation from Molten Silicate: Theory and Experiments

Moderately volatile elements (MVEs) are variably depleted in planetary bodies, reflecting the imprints of nebular and planetary processes. Among MVEs, Na, K, and Rb are excellent tracers for unraveling the history of MVE depletion in planetary bodies because they have similar geochemical behaviors but can be chemically fractionated by evaporation and condensation processes. Furthermore, K and Rb are amenable to high-precision isotopic analyses, which can help constrain the conditions of evaporation and condensation. To quantitatively understand why Na, K, and Rb are depleted in planetary bodies, we have carried out vacuum evaporation experiments from basaltic melt at 1200 and 1400 °C to study their evaporation kinetics and isotopic fractionations. We chose this composition because it is relevant to evaporation from small differentiated planetesimals. The Rb isotopic compositions of the evaporation residues were measured by multicollector inductively coupled plasma mass spectrometry (MC-ICPMS), and the K isotopic compositions were measured along profiles across the residues by secondary ion mass spectrometry (SIMS). In the 1400 °C run products, we found that the concentrations of both K and Rb in the run products decreased from core to rim, which was accompanied by a heavy K isotope enrichment near the surface. This indicates that, in this run, evaporation was limited by diffusion. To use those data quantitatively, we derive analytical equations that describe the evaporation rate and isotopic fractionation associated with diffusion-limited evaporation from a sphere, slab, and cylinder in transient and quasi-steady state regimes. This model is used to tease out the roles that diffusive transport in the melt and evaporation at the melt/gas interface play in setting the elemental depletion and isotopic composition of the residue. Under our experimental conditions, volatility decreases in the order of Na, Rb, and K. Using our experimental results in a thermodynamic model, we have estimated the product γΓ of activity coefficients × evaporation coefficients of Na, Rb, and K. The measured isotopic compositions of the residues are well explained using Rayleigh distillations, whereby the relative volatilities of K and Rb isotopes are given by the square root of their masses. We use our results and previously published data to predict how K and Rb could have been lost as a function of temperature, melt composition, oxygen fugacity, and saturation degree relevant to Vesta’s building blocks. We find that the K and Rb depletions, K/Rb elemental fractionation, and δ 41 K and δ 87 Rb isotopic fractionations of Vesta (as sampled by howardite-eucrite-diogenite (HED) meteorites) are best explained by evaporation of submillimeter size objects for 0.1-10 years at moderate temperatures (~1050 °C) in a medium ~98.8% saturated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaporation Kinetics of Laboratory Generated Secondary Organic Aerosols at Elevated Relative Humidity

Secondary organic aerosols (SOA) dominate atmospheric organic aerosols that affect climate, air quality, and health. Recent studies indicate that, contrary to previously held assumptions, at low relative humidity (RH) these particles are semi-solid and evaporate orders of magnitude slower than expected. Elevated relative humidity has the potential to affect significantly formation, properties, and atmospheric evolution of SOA particles. Here we present a study of the effect of RH on the room-temperature evaporation kinetics of SOA particles formed by ozonolysis of α-pinene and limonene. Experiments were carried out on SOA particles generated, evaporated, and aged at 0%, 50% and 90% RH. We find that in all cases evaporation begins with a relatively fast phase, during which 30% to 70% of the particle mass evaporates in 2 hours, followed by a much slower evaporation rate. Evaporation kinetics at 0% and 50% RH are nearly the same, while at 90% RH a slightly larger fraction evaporates. In all cases, aging the particles prior to inducing evaporation reduces the evaporative losses, with aging at elevated RH leading to more significant effect. In all cases, SOA evaporation is nearly size-independent, providing direct evidence that oligomers play a crucial role in determining the evaporation kinetics.

Environmental Molecular Sciences Laboratory↗

Literature review on impact of glycolate on the 2H evaporator and the effluent treatment facility

Glycolic acid (GA) is being studied as an alternate reductant in the Defense Waste Processing Facility (DWPF) feed preparation process. It will either be a total or partial replacement for the formic acid that is currently used. A literature review has been conducted on the impact of glycolate on two post-DWPF downstream systems - the 2H Evaporator system and the Effluent Treatment Facility (ETF). The DWPF recycle stream serves as a portion of the feed to the 2H Evaporator. Glycolate enters the evaporator system from the glycolate in the recycle stream. The overhead (i.e., condensed phase) from the 2H Evaporator serves as a portion of the feed to the ETF. The literature search revealed that virtually no impact is anticipated for the 2H Evaporator. Glycolate may help reduce scale formation in the evaporator due to its high complexing ability. The drawback of the solubilizing ability is the potential impact on the criticality analysis of the 2H Evaporator system. It is recommended that at least a theoretical evaluation to confirm the finding that no self-propagating violent reactions with nitrate/nitrites will occur should be performed. Similarly, identification of sources of ignition relevant to glycolate and/or update of the composite flammability analysis to reflect the effects from the glycolate additions for the 2H Evaporator system are in order. An evaluation of the 2H Evaporator criticality analysis is also needed. A determination of the amount or fraction of the glycolate in the evaporator overhead is critical to more accurately assess its impact on the ETF. Hence, use of predictive models like OLI Environmental Simulation Package Software (OLI/ESP) and/or testing are recommended for the determination of the glycolate concentration in the overhead. The impact on the ETF depends on the concentration of glycolate in the ETF feed. The impact is classified as minor for feed glycolate concentrations {le} 33 mg/L or 0.44 mM. The ETF unit operations that will have minor/major impacts are chlorination, pH adjustment, 1st mercury removal, organics removal, 2nd mercury removal, and ion exchange. For minor impacts, the general approach is to use historical process operations data/modeling software like OLI/ESP and/or monitoring/compiled process operations data to resolve any uncertainties with testing as a last resort. For major impacts (i.e., glycolate concentrations > 33 mg/L or 0.44 mM), testing is recommended. No impact is envisaged for the following ETF unit operations regardless of the glycolate concentration - filtration, reverse osmosis, ion exchange resin regeneration, and evaporation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Estimation of bare soil evaporation for different depths of water table in the wind-blown sand area of the Ordos Basin, China

Soil surface evaporation is a significant component of the hydrological cycle, occurring at the interface between the atmosphere and vadose zone, but it is affected by factors such as groundwater level, soil properties, solar radiation and others. In order to understand the soil evaporation characteristics in arid regions, a field experiment was conducted in the Ordos Basin, central China, and high accuracy sensors of soil moisture, moisture potential and temperature were installed in three field soil profiles with water-table depths (WTDs) of about 0.4, 1.4 and 2.2 m. Soil-surface-evaporation values were estimated by observed data combined with Darcy’s law. Results showed that: (1) soil-surface-evaporation rate is linked to moisture content and it is also affected by air temperature. When there is sufficient moisture in the soil profile, soil evaporation increases with rising air temperature. For a WTD larger than the height of capillary rise, the soil evaporation is related to soil moisture content, and when air temperature is above 25 °C, the soil moisture content reduces quickly and the evaporation rate lowers; (2) phreatic water contributes to soil surface evaporation under conditions in which the WTD is within the capillary fringe. This indicates that phreatic water would not participate in soil evaporation for a WTD larger than the height of capillary rise. This finding developed further the understanding of phreatic evaporation, and this study provides valuable information on recognized soil evaporation processes in the arid environment.

58 GEOSCIENCES↗

Iodine Distribution During Evaporation of Hanford Waste Treatment Plant Direct Feed Low Activity Waste Effluent Management Facility Simulant

The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream from the off-gas system. The baseline plan for disposition of this stream during full WTP operations is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation, and recycled to the LAW vitrification facility. However, during the Direct Feed LAW (DFLAW) scenario, planned disposition of this stream involves concentrating the condensate in a new evaporator at the Effluent Management Facility (EMF) and returning it to the LAW melter. The LAW melter condensate stream will contain components, e.g. halides and sulfates, that are volatile at melter temperatures, have limited solubility in glass waste forms, and present a material corrosion concern. Further, some minor constituents in the melter condensate, such as volatile organic compounds and iodine, have been found to be at least partially volatile in the EMF. The condensate from the EMF will be sent to the Hanford Effluent Treatment Facility (ETF). The presence of some recalcitrant organics and iodine, as 129I, are expected to be problematic in the ETF. In order to better predict and prepare for the distribution of organics and 129I in the flowsheet, it is key to understand their chemistry and experimentally determine their behavior during evaporation. To do this, modeling and testing were performed to examine the speciation of iodine under relevant conditions, as well as determine partitioning of iodine and the organics in the EMF evaporator. This overall program examines the potential treatment and immobilization of the LAW melter condensate stream to enable alternative disposal. The objective of this task was to (1) perform modeling to determine the speciation and fate of iodine species, (2) prepare a simulant of the LAW Melter Off-gas Condensate expected during DFLAW operations, (3) spike in the key volatile organics and non-radioactive iodine, and (4) demonstrate evaporation in order to predict the final composition of the effluents from the EMF evaporator to aid in planning for their disposition. The results of the modeling of iodine speciation indicate that the iodine is expected to remain in the evaporator pot as iodide and possibly iodate ion if the pH is raised to 11.5-12, which is the planned condition for the EMF. Experimental testing confirmed that the iodide remained in the evaporator concentrate and was below detection limits in all condensate and knock-out pot samples, indicating it was not volatile. The organic nitrile compounds that were added to the simulant were absent from the evaporator feed solution, either lost through evaporation, or more likely, decomposition. The acetone and methylene chloride were below the target values in the feed and condensate samples, and were presumably lost to evaporation or decomposition.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Application of an AREVA Mobile Evaporator Design Used Successfully at NRC Licensed U.S. Commercial Nuclear Sites to Support Hanford Site Operations - 18134

The U.S. Department of Energy (DOE), Office of River Protection (ORP), manages the River Protection Project at the Hanford site in the South Eastern corner of Washington State in the Pacific Northwest of the United States. The mission of the River Protection Project is to retrieve and treat Hanford's tank waste and close the tank farms to protect the Columbia River. The Site Tank Operations Contractor (Washington River Protection Solutions (WRPS)) via its site operations teams creates additional space in the Double Shell Tanks (DSTs) using the site's only remaining operational evaporator - 242-A. The current 242-A Evaporator has long been identified as a potential single point of failure that in the event of a major breakdown, could significantly impact retrieval operations at the Hanford Site. Areva has experience both on the Hanford site as an integrated subcontractor to the mission and in the design, procurement and construction of a mobile forced circulation evaporator unit designed to be used on Nuclear Regulatory Commission commercial nuclear utility sites. The mobile unit has been used at the following nuclear power plants: SONGS, Salem, Davis Besse, Waterford and Palo Verde. It was designed to take spent Water-EDTA based chemical cleaning solvent and evaporate water off to reduce the volume of waste required to go through downstream processes. It was further designed to fit inside ISO shipping containers. A multi-step approach will be used to: 1. review lessons learned from the previous DOE study for deploying a mobile evaporator on the Hanford sit, 2. evaluate the proposed waste streams and the required throughput and waste arising, sizing the evaporator appropriately, 3. develop a concept design requirements document for the use of a customized evaporator to meet the Hanford need 4. Design, and build a mobile evaporator and 5. Test, install and commission at a site to be agreed with WRPS/DOE. With an overall budget for the approach described of around $35 m, an operational evaporator could be delivered to site in 18-24 months from the approval of a detailed design package. Potential befits include the elimination of the 242-A evaporator as a single point failure, the creation of additional DST tank space and the elimination of the need to stage waste at the 242-A evaporator by moving the mobile unit to a location where is could be deployed at or close to the tank such as in 200W. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Technetium-99 Behavior in Low-Temperature, Low-Pressure Evaporation Systems at the Hanford Site - 18461

This paper seeks to provide a technical basis for predicting the behavior of Technetium-99 (Tc-99) in the Effluent Management Facility (EMF) evaporator during the Direct Feed Low-Activity Waste (DFLAW) mission at the Hanford Site. This is done by using the 242-A Evaporator and the DM10 Melter System evaporator as analogues for the predicted design and operating strategy of the EMF evaporator. The focus of this investigation is to establish how Tc-99 behavior coincides with the behavior of several process variables (e.g. feed Tc-99 concentrations, feed sources, extent of evaporative concentration) associated with low-temperature, low-pressure evaporator operations. The primary measure of Tc-99 behavior was the partitioning of Tc-99 from the feed stream into the condensate stream (i.e. boil-off) of the evaporators. Analysis of 242-A and DM10 Melter System evaporator data allowed for the identification of the following trends regarding Tc-99 behavior in low-temperature, low-pressure evaporator systems: Tc-99 partitions minimally from the feed to the condensate stream and Tc-99 partitions consistently across a variety of operating and feed conditions. Given the similarities in design and operating strategies between the studied evaporator systems and the EMF evaporator, it is reasonable to suggest that these trends can be used to aid in planning for future EMF operations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Investigating Evaporation in Gas Diffusion Layers for Fuel Cells with X-ray Computed Tomography

Understanding evaporation in porous media and the associated water distribution for a given saturation is critical for optimizing many different technologies including polymer-electrolyte fuel cells. In these devices, heat and mass-transport are coupled due to the two-phase transport of water and operating temperatures from subzero to 80°C. Especially critical is understanding phase change in the mixed wettability, carbon gas-diffusion layers (GDLs). While previous works have measured evaporation rates empirically for a given saturation, there remains a need to explore the mechanisms governing evaporation, which are tied directly to the internal water distribution. Here in this paper, liquid-water evaporation rates in GDLs are measured in situ using synchrotron X-ray computed tomography (CT). X-ray CT allows visualizing the evaporating water-front location and interfacial water/air surface area, thereby enabling true surface-area based evaporation rates. It is found that the overall specific evaporation rate is essentially constant as a function of saturation and that the water/air interfacial area scales almost linearly with saturation. To isolate transport and kinetic contributions to the overall evaporation rate, we systematically varied gas flow rate and composition. A three-dimensional mathematical model with direct meshes of liquid-water evaporation fronts from the X-ray CT studies allowed for the determination that the evaporation is transport limited. The overall results provide insight into evaporation phenomena in porous media.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Optimization of lithium vapor box divertor evaporator location on NSTX-U using SOLPS-ITER

Commercial fusion reactors will be faced with extremely high divertor target heat fluxes that will require mitigation. Simulations of detachment in an NSTX-U scenario projected to have 92 MW/m 2 unmitigated peak target heat flux are presented, which reaches sub-10 MW/m 2 target heat flux using a highly dissipating lithium vapor box divertor design. The lithium vapor box is a detached divertor design which employs lithium vapor evaporation and condensation to contain lithium below the X-point. Previous SOLPS modeling has indicated a lithium vapor box can reduce the heat flux down to 10 MW/m 2 via simultaneous evaporation from the Private Flux Region (PFR) and the Common Flux Region (CFR) sides of the vapor box. It is found here that PFR evaporation has improved access to the separatrix leading to significantly more efficient power dissipation than CFR evaporation. Simulations of target evaporation with an evaporation distribution that is self-consistent with the temperature of a Capillary Porous System with Fast flowing liquid lithium (CPSF) could reach n Li / n e ~ 0.025-0.030 at the Last Closed Flux Surface (LCFS) depending on the liquid metal flow speeds and lithium sputtering yield, while PFR-side evaporation can reach acceptable heat fluxes with n Li / n e ~ 0.038 at the LCFS. However, PFR evaporator performance can be improved if the target is allowed to be hot enough such that it reflects lithium, reaching n Li / n e ~ 0.028 and reducing required lithium evaporation. Ultimately PFR evaporation and target evaporation are found to have similar ability to produce acceptable heat flux solutions with minimal upstream concentration.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Surface Crust Formation Controls Evaporation Kinetics of Secondary Organic Aerosols

Gas-particle partitioning is critical for the evolution of secondary organic aerosols (SOA) in the atmosphere. SOA particles evaporate more slowly than expected at nearly size-independent rates, but the underlying mechanism remains controversial. Here, in this study, we apply kinetic multilayer modeling to simulate evaporation of α-pinene SOA, demonstrating that surface crust formation, emerging from accumulation of low-volatility compounds at the particle surface, leads to slow evaporation and reduced size dependence of the evaporation rate. While evaporation induced by decomposition of oligomers would naturally lead to size-independent evaporation rates, we observe and simulate nearly size-independent slow evaporation of polyethylene glycol mixture particles containing polymeric species that do not decompose, confirming the relevance of composition-dependent diffusivity for size-independent, slow evaporation. Slow evaporation of limonene SOA was also observed in environmental chamber experiments, and model simulations demonstrate strong surface crust formation with bulk diffusivity being depressed by up to 5 orders of magnitude compared to the inner bulk. We present experimental evidence using a surface-based mass spectrometry technique that shows that the particle surface becomes enriched in high molecular weight compounds upon evaporation of monomers. Our findings imply that viscous surface crusts may also limit the growth and chemical transformation of SOA particles, influencing their impacts on air quality and climate.

heterogeneous chemistry↗

Evaluating Enhanced Reservoir Evaporation Losses From CMIP6‐Based Future Projections in the Contiguous United States

Abstract Enhanced reservoir evaporation has become an emerging concern regarding water loss, especially when compounded with the ever‐increasing water demand. In this study, we evaluated the evaporation rates and losses for 678 major reservoirs (representing nearly 90% of total storage capacity) in the Contiguous United States over historical baseline (1980–2019), near‐term (2020–2039), and mid‐term (2040–2059) future periods. The evaporation rate was estimated using the Lake Evaporation Model (LEM), an advanced lake evaporation model that addresses both heat storage and fetch effects, driven by multi‐ensemble downscaled Coupled Model Intercomparison Projects 6 (CMIP6) projections under the SSP585 emission scenario. The results project that the evaporation loss may increase by 2.5 × 10 7 m 3 /yr through the research period (1980–2059). Among all regions, the Rio Grande is projected to have the largest increasing rate in the near‐term and mid‐term future, with values of 7.11% of 10.25%, respectively. At the seasonal scale, the most significant increase in the evaporation rate is projected during the fall. The evaporation is projected to increase faster than the streamflow over many of the regions in the southwestern US during the summer/fall, suggesting that the shortage of water will be further exacerbated. The climate models contribute the most to the variance, as compared to the other components related to the projection of evaporation losses (e.g., hydrological model, downscaling method, and historical meteorological data set). These findings demonstrate the need to consider accelerated water loss through open water evaporation in long‐term water resources planning across various spatiotemporal scales.

54 ENVIRONMENTAL SCIENCES↗