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At least 73 records · Page 4

Source Contributions to Fine Particulate Matter and Attributable Mortality in India and the Surrounding Region

Fine particulate matter (PM 2.5 ) is a leading mortality risk factor in India and the surrounding region of South Asia. This study evaluates the contribution of emission sectors and fuels to PM 2.5 mass for 29 states in India and 6 surrounding countries (Pakistan, Bangladesh, Nepal, Bhutan, Sri Lanka, and Myanmar) by combining source-specific emission estimates, stretched grid simulations from a chemical transport model, high resolution hybrid PM 2.5 , and disease-specific mortality estimates. We find that 1.02 (95% Confidence Interval (CI): 0.78-1.26) million deaths in South Asia attributable to ambient PM 2.5 in 2019 were primarily from three leading sectors: residential combustion (28%), industry (15%), and power generation (12%). Solid biofuel is the leading combustible fuel contributing to the PM 2.5 -attributable mortality (31%), followed by coal (17%), and oil and gas (14%). State-level analyses reveal higher residential combustion contributions (35%-39%) in states (Delhi, Uttar-Pradesh, Haryana) with high ambient PM 2.5 (>95 µg/m 3 ). The combined mortality burden associated with residential combustion (ambient) and household air pollution (HAP) in India is 0.72 million (95% CI:0.54-0.89) (68% attributable to HAP, 32% attributable to residential combustion). Our results illustrate the potential to reduce PM 2.5 mass and improve population health by reducing emissions from traditional energy sources across multiple sources in South Asia.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Modeling Riverine Dissolved and Particulate Organic Carbon Fluxes from Two Small Watersheds in the Northeastern United States

The coupled carbon (C) cycle across terrestrial and aquatic environments at the watershed scale has been identified as an important, but poorly constrained component of the global carbon budget. Here, we extended Soil and Water Assessment Tool (SWAT) with coupled riverine particulate organic carbon (POC) and dissolved organic carbon (DOC) modules (referred to as SWAT-C hereafter). Results show that SWAT-C reproduced daily POC and DOC fluxes well in two watersheds in the Northeastern United States. We found that SWAT-C tended to underestimate high flows and peak DOC and POC fluxes. Uncertainty analysis indicated flux uncertainties associated with POC and DOC simulation were larger than those for flow simulation. Sensitive parameters controlling POC and DOC biogeochemical processes were identified along with how these parameters influence mechanisms underlying C cycling. We anticipate that the tool developed and applied here will inform C related ecosystem services in watershed assessment and planning.

Dissolved organic carbon, Particulate organic carb↗

Impacts of engine lubrication oil-derived ash on soot oxidative reactivity on a catalytic gasoline particulate filter

Characterizing soot oxidation kinetics is crucial for understanding how gasoline particulate filters (GPFs) perform both in terms of filtration efficiency and pressure drop. The most common method for measuring soot oxidative reactivity is thermogravimetric analysis (TGA). Because TGA is an offline method, it may inaccurately predict how soot oxidizes on a GPF, especially if a catalytic washcoat is present that may enhance oxidation rates through surface interactions as the soot loads on the filter. In this work, a novel in-situ soot oxidative reactivity measurement method was developed. The method involved loading a catalytic GPF under high temperature conditions conducive to soot oxidation and measuring the filtration efficiency of 100 nm particles. A correlation was made between filtration efficiency and loaded soot mass on the filter to allow calculation of the soot oxidation rate. The method was evaluated in experiments using a 2.0 L gasoline direct injection (GDI) engine with three oils of varying additive packages, including an oil with a high zinc dialkyldithiophosphate (ZDDP) concentration, a non-additive, pure poly-alpha olefin (PAO) oil, and an oil with a high concentration of calcium sulfonate. Calculated specific soot oxidation rates ranged from ~0.06–0.6 min –1 and showed strong dependence on GPF inlet gas temperature and lubrication oil additive type. The results clearly demonstrated a catalytic effect of calcium-containing ash particles. Reactivity of soot produced by the engine running with the high calcium containing lubrication oil was increased. Similarly, the results indicated that the catalytic washcoat on the filter increased soot oxidation rates on-filter, especially at low soot loading. Conversely, the ZDDP oil additive exhibited a reactivity inhibiting effect, resulting in lower soot oxidation rates. Finally, this work represents the first known in-situ soot oxidative reactivity measurements on a GPF and elucidates the effect of lubrication oil additives and catalytic washcoat on oxidation rate.

42 ENGINEERING↗

Ability of Particulate Matter Index to describe sooting tendency of various gasoline formulations in a stratified-charge spark-ignition engine

This study investigates the ability of Particulate Matter Index (PMI) to describe the sooting behavior of various gasoline formulations in a stratified-charge (SC) spark-ignition engine. Specifically, the engine was operated at 2000 rpm with an intake pressure of 130 kPa where soot formation is known to primarily occur in the bulk gases. Exhaust soot emissions were measured for nine test fuels at various exhaust gas recirculation levels. A comparison between measured soot levels and PMI shows that PMI is a relatively poor predictor of the sooting tendency of the tested fuels under lean SC combustion. Among the fuels, three fuels, namely the diisobutylene blend, High Olefin, and E30 fuels exhibit measured soot behavior opposite of that predicted by PMI. Optical diagnostics were utilized to further investigate the in-cylinder phenomena for these three fuels. Analysis of natural luminosity and diffused back-illumination extinction imaging suggests that fuel-induced differences in the amount of soot formed are responsible for a majority of the discrepancy in measured versus predicted sooting tendency. Fuel-induced differences in soot oxidation and spray development seem to play minor roles. Because the combustion and air-fuel mixing processes for lean SC combustion are different from conventional stoichiometric operation it is hypothesized that the PMI correlation needs to be modified to account for differences in stoichiometric air-fuel ratio and level of oxygenation between fuels. Furthermore, the role of fuel volatility in PMI possibly needs to be de-emphasized for SC operation with fuel injection into compression-heated gases.

42 ENGINEERING↗

Responses of gaseous sulfuric acid and particulate sulfate to reduced SO 2 concentration: A perspective from long-term measurements in Beijing

SO 2 concentration decreased rapidly in recent years in China due to the implementation of strict control policies by the government. Particulate sulfate ( p S O 4 2 - ) and gaseous H 2 SO 4 (SA) are two major products of SO 2 and they play important roles in the haze formation and new particle formation (NPF), respectively. We examined the change in p S O 4 2 - and SA concentrations in response to reduced SO 2 concentration using long-term measurement data in Beijing. Simulations from the Community Multiscale Air Quality model with a 2-D Volatility Basis Set (CMAQ/2D-VBS) were used for comparison. From 2013 to 2018, SO 2 concentration in Beijing decreased by ~81% (from 9.1 ppb to 1.7 ppb). p S O 4 2 - concentration in submicrometer particles decreased by ~60% from 2012–2013 (monthly average of ~10 μg·m - 3 ) to 2018–2019 (monthly average of ~4 μg·m - 3 ). Accordingly, the fraction of p S O 4 2 - in these particles decreased from 20–30% to <10%. Increased sulfur oxidation ratio was observed both in the measurements and the CMAQ/2D-VBS simulations. Despite the reduction in SO 2 concentration, there was no obvious decrease in SA concentration based on data from several measuring periods from 2008 to 2019. This was supported by the increased SA:SO 2 ratio with reduced SO 2 concentration and condensation sink. NPF frequency in Beijing between 2004 and 2019 remains relatively constant. Finally, this constant NPF frequency is consistent with the relatively stable SA concentration in Beijing, while different from some other cities where NPF frequency was reported to decrease with decreased SO 2 concentrations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Responses of particulate and mineral-associated organic carbon to temperature changes and their mineral protection mechanisms: A soil translocation experiment

Mineral protection mechanisms are important in determining the response of particulate organic carbon (POC) and mineral-associated organic carbon (MAOC) to temperature changes. However, the underlying mechanisms for how POC and MAOC respond to temperature changes are remain unclear. Here, by translocating soils across 1304 m, 1425 m and 2202 m elevation gradient in a temperate forest, simulate nine months of warming (with soil temperature change of +1.41 °C and +3.91 °C) and cooling (with soil temperature change of −1.86 °C and −4.20 °C), we found that warming translocation significantly decreased POC by an average of 10.84 %, but increased MAOC by an average of 4.25 %. Conversely, cooling translocation led to an average increase of 8.64 % in POC and 13.48 % in MAOC. Exchangeable calcium (Ca exe ) had a significant positive correlation with POC and MAOC during temperature changes, and Fe/Al-(hydr)oxides had no significant correlation or a significant negative correlation with POC and MAOC. Our results showed that POC was more sensitive than MAOC to temperature changes. Ca exe mediated the stability of POC and MAOC under temperature changes, and Fe/Al-(hydr)oxides had no obvious protective effect on POC and MAOC. Our results support the role of mineral protection in the stabilization mechanism of POC and MAOC in response to climate change and are critical for understanding the consequences of global change on soil organic carbon (SOC) dynamics.

Mineral protection↗

Ducted Fuel Injection And Cooled Spray Technologies For Particulate Control In Heavy-duty Diesel Engines (Final Report)

Cooled Spray (CS) and Ducted Fuel Injection (DFI) are in-cylinder technologies for diesel engines that can reduce particulate matter and soot emissions and data has been published showing that these technologies can reduce soot emissions by 75-100% for some engines at some operating conditions. However, little is known about scaling the devices for engine size. Additionally, the performance of either technology over the engine duty cycle has not been explored. This project addresses both of these points through single-cylinder engine investigations. The objectives of this project are to provide details about dimensional scaling of these devices and to demonstrate 75% PM reduction over a range of operating conditions on a single-cylinder engine. Two engines were used for this project: a 125mm bore optically accessible engine at Sandia National Laboratories and a 168mm bore metal engine at Southwest Research Institute. The optical engine was used to study the performance of DFI and CS inserts for a large injector orifice diameter injector that is characteristic of a locomotive engine and to perform scaling studies for DFI. The metal engine was used to perform scaling and alignment studies for CS and to evaluate the technology for both EGR and non-EGR engines over the engine operating map. Modifications were required for both engines to accept the prototype inserts being tested. The optical engine required a new fuel injector, cylinder head and piston so that tests could be run at the pressures and engine speeds required. Additionally, a novel rotating stage was designed for the optical engine to simplify alignment of the modules. The metal engine required a modified cylinder head to accept CS inserts and a modified piston to provide additional space around the fuel injector for the CS inserts. Tests on the optical engine showed that DFI reduces PM emissions for both small injector orifices (0.170mm diameter) and large injector orifices (0.290mm). For high load testing, the DFI modules were not as effective as at low load testing, but it was acknowledged that minimal geometric optimization was performed and more improvements may be possible. Comparing DFI to CS and conventional diesel combustion (CDC), DFI performed better than CS or CDC. The CS geometries used in these studies may not be ideal for that engine and additional modifications likely would improve performance. Tests on the metal engine showed PM reductions as high has 80% at some operating conditions with duty-cycle PM reductions of ~50% for EGR and non-EGR configurations. The CS testing on the metal engine showed that chamfering of the fuel passage inlet either through hydro-erosion or mechanical grinding provided significant improvements in the PM reduction capabilities of the insert. Additionally, alignment sensitivities were explored and the data show that the tolerance to misalignment is approximately 0.05 to 0.1mm for the inserts that were studied here. Air-fuel ratio was shown to be important in the effectiveness of the CS inserts. In several tests, it was shown that the CS inserts are more effective at reducing the PM for high-AFR operating conditions compared to low AFR conditions. In summary, multiple designs were evaluated on both engines. It was found that for the conditions and configurations studied here, a fuel passage diameter of ~2.5mm performed best overall. Significant duty-cycle PM reductions are possible using these technologies and sensitivities to AFR, alignment fuel passage diameter and inlet fuel passage shaping were explored and are reported here. More PM reduction may be possible with improved geometric design and attention to alignment practices.

02 PETROLEUM↗

Impact of Biofuel Blending on Hydrocarbon Speciation and Particulate Matter from a Medium-Duty Multimode Combustion Strategy

The U.S. Department of Energy’s Co-Optima initiative simultaneous focused on diversifying fuel sources, improving efficiency, and reducing emissions through using novel combustion strategies and sustainable fuel blends. For medium-duty/heavy-duty diesel engines, research in this area has led to the development of a multimode strategy that uses premixed charge compression ignition (PCCI) at low loads and conventional diesel combustion (CDC) at mid–high loads. The aim of this study was to understand how emissions were impacted when using PCCI instead of CDC at low loads and switching to an oxygenated biofuel blend. It provides a detailed speciation of the hydrocarbon (HC) and particulate matter (PM) emissions from a multimode medium-duty engine operating at low loads in PCCI and CDC modes and high loads in CDC. The effect of the oxygenated biofuel blend on emissions was studied at all three mode–load conditions using #2 ULSD and a bio-derived fuel (25% hexyl hexanoate (HHN)) blended in #2 ULSD. The PCCI mode effectively decreased NOx, total HC, and PM/PN emissions, with a substantial decrease in larger particles (≥50 nm). A PM/PN reduction was observed at high loads with the 25% HHN fuel. While the total HC emissions were not impacted by fuel type, the detailed HC analysis exposed changes in the HC’s composition.

09 BIOMASS FUELS↗

Soil Particulate Organic Matter is Related to Ericoid Mycorrhizal Shrubs, not Ectomycorrhizal Trees, in a Temperate Forest

Mycorrhizal associations are key drivers of soil biogeochemistry, but previous studies have focused almost exclusively on ectomycorrhizal (EcM) and arbuscular mycorrhizal (AM) associations. Ericoid mycorrhizal (ErM) shrubs frequently occur in forest understories and are expanding in response to disturbance, but are rarely considered in biogeochemical frameworks. We investigated the relationships of understory ErM shrubs and overstory trees on carbon (C) and nitrogen (N) in soil organic matter fractions in a southern Appalachian temperate forest. We sampled the 0–10 cm mineral soil layer from 43 plots at the Coweeta Hydrologic Laboratory, across gradients in overstory EcM dominance and understory ErM shrub biomass. Soil C:N ratios increased with both increasing EcM dominance and increasing ErM shrub biomass. However, total particulate organic matter (POM) C, and the proportion of C and N held in POM increased with increasing ErM shrub biomass, but not with increasing EcM dominance. In contrast, mineral-associated organic matter (MAOM) C and N were negatively associated with EcM dominance, but were not related to ErM shrubs. Our findings suggest that ErM shrubs facilitate POM formation while AM trees promote MAOM formation. Because ErM shrub biomass represents a small fraction of total forest biomass, our work provides evidence that ErM shrubs have an outsized effect on soil organic matter, which advocates for their inclusion in mechanistic studies and biogeochemical frameworks.

Bonilla, Kayla A. [University of Georgia, Athens, ↗

Potential reductions in fine particulate matter and premature mortality following implementation of air pollution controls on coal-fired power plants in India

Coal-fired power plants (CFPPs) account for > 70% of electricity generation in India, but < 5% of facilities have installed technologies for sulfur dioxide (SO 2 ) and nitrogen oxide (NO X ) removal. Emissions of these pollutants lead to the formation of fine particulate matter (PM 2.5 ) and an increased risk of premature mortality for exposed populations. Here, we use a nested version of the GEOS-Chem global chemical transport model (0.5° × 0.625° resolution) for India to estimate reductions in PM 2.5 concentrations that could have been achieved by implementing existing emission control technologies like flue-gas desulfurization (FGD) and/or selective catalytic reduction (SCR). We quantify the associated burden of disease using the integrated exposure response (IER) and global exposure mortality model (GEMM) functions and compare the costs of premature mortality to those for FGD installation. Model simulations for 2010 suggest installation of FGD would have reduced mean annual PM 2.5 concentrations across India by 8%, compared to 3% with SCR installation, and 11% with both FGD and SCR. A 7–28% reduction in PM 2.5 was simulated for local communities closest to CFPPs (same model grid cell), leading to up to 17% reduction in annual premature mortality. Overall, more than 0.21–0.48 million premature deaths would have been avoided over a 10-year period if FGD had been implemented on all CFPPs, compared to 0.09–0.21 million with SCR and 0.22–0.72 million with both FGD and SCR. Benefits associated with such actions are approximately $\$18.1$–$\$604$ billion USD per year, which is equivalent to ~ 0.44 to 10% of India’s GDP. These results suggest that monetary benefits from avoided premature mortality far outweigh the capital and operational costs of FGD and/or SCR installation of $\$19.5$ billion and/or $\$32.8$ billion per year, respectively. This information is essential because the high costs of installation and operation are often given as reasons for delaying installation and commissioning. Finally, we conclude that policy actions to control air pollution from CFPPs are economically justifiable.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Particulate Fuel Modeling of MC 2 -3 using Iterative Local Spatial Self-shielding Method

We report a new spatial self-shielding method for particulate fuels has been developed based on disadvantage factors and implemented in the MC 2 -3 code. This method named the iterative local spatial self-shielding (ILSS) method considers the shadowing effect of randomly distributed particles on spatial self-shielding in particles through a homogenized composition region added outside the particle of interest at the center. The self-shielded cross sections of the central particle are determined iteratively since they are used in determining the cross sections of the homogenized composition region. The ILSS method was verified for infinite stochastic medium problems of single and multiple types of particles, VHTR unit cell problems, and HTTR assembly problems. The verification test results show that the ILSS method accurately predicts the stochastic particle shadowing effect and reaction rates in particles, whereas the regular array model and the stochastic collision probability method underpredict the particle shadowing effect and overestimate reaction rates in particles.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An extended three-field principle to scale-bridge the granular micromechanics of polymer-bonded particulate materials

Observed phenomena of damage, viscoelasticity, and viscoplasticity in polymer-bonded particulate materials (PBPM), like polymer-bonded explosive (PBX), are accommodated in a scale-bridging constitutive model based on granular micromechanics. An extended three-field variational principle with min - max optimization problem is introduced to homogenize the bonded aggregates’ grain-scale contact mechanics. Similarly to prior applications of a three-field principle, volume constraints are invoked to embed microscale-to-macroscale correspondences for kinematic and static volumetric measures, like mean strain and its energy-conjugate stress invariant. Unlike prior applications, our three-field principle realizes a strain-driven model for effective constitutive behavior due to bonded intergranular contact. In conclusion, the resultant micro-sphere integration-based homogenization is demonstrated in comparison to existing publicly-available measurements to capture the extreme tension/compression constitutive asymmetry exhibited by PBPMs (specifically PBX-9501) during material softening.

42 ENGINEERING↗

Self-healing carbon fiber/epoxy laminates with particulate interlayers of a low-melting-point alloy

In order to prolong the service life of fiber-reinforced polymer composites, the implementation of self-healing ability with the micro-encapsulated healing agent has been extensively studied. However, such microcapsule-based self-healing composites typically suffer from degraded mechanical properties due to the liquid-phase inclusions, thereby limiting their proliferation. Here, in this study, a low-melting-point alloy is utilized as the particulate inclusions of carbon fiber/epoxy laminated composites. Field's Metal particles (melting point: 62 °C) are distributed between woven carbon fiber preforms followed by the resin impregnation to realize laminated composites with a Field's Metal-enhanced interlayer(s). The resulting laminated composites demonstrate the autonomic repair of interlaminar failure with a 40 % of healing efficiency. Most of all, the mechanical properties of these self-healing laminated composites are comparable to the conventional laminated composites attributed to the rigid inclusions that can be compressed to increase the fiber volume. Since the Field's Metal particle inclusions can bestow polymer composites with self-healing ability and the potential increase in mechanical properties, Field's Metal-enhanced fiber-reinforced polymer composites are expected to unlock the practical utility of self-healing composites.

A. polymer-matrix composites (PMCs)↗

Dicarboxylic acid emissions from a GDI engine equipped with a catalytic gasoline particulate filter

Dicarboxylic acids play an important role in atmospheric chemistry, yet their emissions from primary sources, such as internal combustion engines, has not been extensively studied. In this paper, KOH impregnated quartz filters were loaded with exhaust gases from a gasoline direct injection (GDI) engine equipped with a catalytic gasoline particulate filter (GPF). All filters were analyzed for carboxylic and dicarboxylic acids using a derivatized gas chromatography-mass spectroscopy method. Exhaust gas was sampled from pre-GPF and post-GPF locations to determine the performance of the GPF regarding acid conversion. Lean and stoichiometric engine modes were considered with non-oxygenated gasoline and 10% splash blended ethanol in gasoline (E10) to examine the impact of stoichiometry and fuel type. Acid emissions represented as much as 0.51% of total unburned hydrocarbon emissions for total monocarboxylic acids and as much as 0.40% for total dicarboxylic acids. Individual acid concentrations were as high as 38 mg/kg-fuel for monocarboxylic acids and as high as 29 mg/kg-fuel for dicarboxylic acids. Overall, the study found that fuel oxygenates had mixed impact on the acid emissions. Engine-out monocarboxylic acids were reduced when using the E10 fuel by approximately 30–45% for the stoichiometric condition and increased marginally for the lean condition. Dicarboxylic acid emissions were generally insensitive to ethanol content. However, the engine condition significantly affected the acid emissions. Lean operation produced a factor of two to an order of magnitude higher emissions rates of both monocarboxylic and dicarboxylic acids than the stoichiometric condition. The catalytic GPF eliminated between 80 and 92% of the acids emitted from the engine, allowing some acids to be emitted into the environment.

42 ENGINEERING↗

Changing chemistry of particulate manganese in the near- and far-field hydrothermal plumes from 15°S East Pacific Rise and its influence on metal scavenging

Dissolved Mn(II) in the hydrothermal plume is known to be microbially oxidized to form Mn(III/IV) oxides, and the Mn oxides scavenge other trace elements in seawater. In the GEOTRACES GP16 cruise, dissolved Mn (dMn) and particulate Mn (pMn) were found to be transported over 4000 km westwards from the Southern Eastern Pacific Rise. Previous studies in this plume showed different removal rates of dMn and pMn as well as pMn size distribution between the near-field (<80 km from the ridge axis) and far-field (>80 km) plumes. In order to understand Mn cycling in these plumes, spatial distribution, oxidation states, and mineral structures of Mn in small size fraction (SSF; 0.8–51 μm) and large size fraction (LSF; >51 μm) particles from the near-field and far-field plumes were examined using micro X-ray fluorescence spectrometry (μ-XRF), X-ray absorption near-edge structure spectroscopy (XANES), chemical species mapping, and extended X-ray absorption fine-structure spectroscopy (EXAFS). In the near-field plume, pMn in the SSF is dominated by oxidized Mn with Mn(III) fractions of ~30%. They are a mixture of δ-MnO 2 and triclinic birnessites that is known to be formed as a result of autocatalytic Mn(II) oxidation at the surface of freshly-formed δ-MnO2, suggesting that both microbial and autocatalytic Mn oxidation occur in the near-field plume. The LSF pMn in the near-field plume is also oxidized and often found in large aggregates several hundreds of μm in size. These aggregates settle out in the near-field and during transport, and are not found in the far-field plume. In the far-field plume where Mn oxides are not newly formed, pMn in the SSF is oxidized, but their Mn(III) fractions are smaller than in the near-field pMn. Unlike the SSF, the far-field plume LSF pMn is dominated by reduced Mn, implying very slow aggregation of pMn in the far-field plume. The different characteristics of pMn between the near-field and far-field plumes affect its scavenging of other trace elements. In the near-field plume, Co, Mo, 231 Pa are associated with pMn, but not in the far-field plume. 231 Pa is adsorbed to pFe rather than pMn in the far-field plume, and Pb is adsorbed to pFe in the entire plume. The result shows that freshly-formed Mn oxides in the near-field plume have higher scavenging capacity than the far-field plume pMn. Our findings suggest that the mineralogical age of Mn oxides may be an important parameter that controls the scavenging of many other trace elements and isotopes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Toward reducing uncertainty quantification costs in DEM models of particulate flow: Testing simple, sensitivity-based, forward uncertainty propagation techniques

The performance of two conceptually-simple uncertainty quantification techniques are tested against the rigorous nested-loop sampling technique of Roy and Oberkampf (Comput Methods Appl Mech Eng, 200: 2131–2144, 2011) (herein called full-sampling) using two very small-scale DEM-based models of particulate flow (one gas-solid flow and one granular flow). The first simplified forward uncertainty propagation technique, reduced-sampling, uses a sensitivity analysis to eliminate uncertain inputs that have little impact on the model output prior to nested-loop sampling. The second technique, boundary-sampling, uses a sensitivity analysis to inform the selection of two bounding cases for each key model output. In conclusion, the uncertainties in the model outputs obtained via the reduced- and boundary-sampling methods agree well with those from full-sampling for both the gas-solid and granular flow models while yielding computational savings of 65–75% (reduced sampling) and 94–97% (boundary sampling).

42 ENGINEERING↗

Particulate plutonium released from the Fukushima Daiichi meltdowns

Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O 2 nanoparticles, <~10 nm, one of which is enriched in Pu adjacent to fragments of Zr-cladding. The isotope ratios, 235 U/ 238 U, 240 Pu/ 239 Pu, and 242 Pu/ 239 Pu, of the CsMPs were determined to be ~0.0193, ~0.347, and ~0.065, respectively, which are consistent with the calculated isotopic ratios of irradiated-fuel fragments. Thus, considering the regional distribution of CsMPs, the long-distance dispersion of Pu from FNDPP is attributed to the transport by CsMPs that have incorporated nanoscale fuel fragments prior to their dispersion up to 230 km away from the Fukushima Daiichi reactor site.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗