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At least 667 records · Page 37

Coupled Interfacial and Bulk Kinetics Govern the Timescales of Multiphase Ozonolysis Reactions

Chemical transformations in aerosols impact the lifetime of particle phase species, the fate of atmospheric pollutants, and both climate- and health-relevant aerosol properties. Timescales for multiphase reactions of ozone in atmospheric aqueous phases are governed by coupled kinetic processes between the gas phase, the particle interface, and its bulk, which respond dynamically to reactive consumption of O 3 . However, models of atmospheric aerosol reactivity often do not account for the coupled nature of multiphase processes. Herein, to examine these dynamics, we use new and prior experimental observations of aqueous droplet reaction kinetics, including three systems with a range of surface affinities and ozonolysis rate coefficients ( trans -aconitic acid (C 6 H 6 O 6 ), maleic acid (C 4 H 4 O 4 ), and sodium nitrite (NaNO 2 )). Using literature rate coefficients and thermodynamic properties, we constrain a simple two-compartment stochastic kinetic model which resolves the interface from the particle bulk and represents O 3 partitioning, diffusion, and reaction as a coupled kinetic system. Our kinetic model accurately predicts decay kinetics across all three systems, demonstrating that both the thermodynamic properties of O 3 and the coupled kinetic and diffusion processes are key to making accurate predictions. An enhanced concentration of adsorbed O 3 , compared to gas and bulk phases is rapidly maintained and remains constant even as O 3 is consumed by reaction. Multiphase systems dynamically seek to achieve equilibrium in response to reactive O 3 loss, but this is hampered at solute concentrations relevant to aqueous aerosol by the rate of O 3 arrival in the bulk by diffusion. As a result, bulk-phase O 3 becomes depleted from its Henry's law solubility. This bulk-phase O 3 depletion limits reaction timescales for relatively slow-reacting organic solutes with low interfacial affinity (i.e., trans-aconitic and maleic acids, with k rxn ≈ 10 3 -10 4 M -1 s -1 ), which is in contrast to fast-reacting solutes with higher surface affinity (i.e., nitrite, with k rxn ≈ 10 5 M -1 s -1 ) where surface reactions strongly impact the observed decay kinetics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Late Holocene Cliff Retreat in Del Mar, CA, Revealed From Shore Platform 10 Be Concentrations and Numerical Modeling

Rocky coast cliff retreat presents a hazard to coastal communities and infrastructure that is potentially amplified under rising sea level conditions, among other factors. Unfortunately, constraints on retreat rates are typically limited to those derived from imagery and maps spanning the last ~100 years. Here, we use a newly developed coupled model of shore platform profile evolution and cosmogenic radionuclide production that considers the influence of relative sea level (RSL) rise, weathering, material resistance, and wave height decay to model cliff retreat over millennial timescales and its potential drivers in Del Mar, California. We demonstrate the ability to use topographic and bathymetric measurements from a narrow shore platform along with a limited data set of nine cosmogenic 10Be concentrations extending ~125 m from the cliff base to obtain modeled cliff retreat rates that steadily range from 5.0 to 12.5 cm yr -1 over the last two millennia until 100 years before present. These rates are consistent with modern retreat rates of about 2–19 cm yr -1 here. RSL rise in Southern California remained relatively constant during the late Holocene, potentially explaining the relatively stable modeled cliff retreat rate over this time. We also explore the relative influence of weathering, material resistance, and wave erosion efficacy and find that both weathering and wave-driven erosion are necessary to replicate the measured data at this location, with the latter exerting a stronger control on model acceptance, suggesting that waves may provide a possible mechanism by which RSL rise may influence coastal cliff erosion in southern California.

58 GEOSCIENCES↗

Imaging multiphoton ionization dynamics of CH 3 I at a high repetition rate XUV free-electron laser

XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core–hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (~75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems.

Optics↗

Performance of the ATLAS RPC detector and Level-1 muon barrel trigger at √(s)=13 TeV

The ATLAS experiment at the Large Hadron Collider (LHC) employs a trigger system consisting of a first-level hardware trigger (L1) and a software-based high-level trigger. The L1 muon trigger system selects muon candidates, assigns them to the correct LHC bunch crossing and classifies them into one of six transverse-momentum threshold classes. The L1 muon trigger system uses resistive-plate chambers (RPCs) to generate the muon-induced trigger signals in the central (barrel) region of the ATLAS detector. The ATLAS RPCs are arranged in six concentric layers and operate in a toroidal magnetic field with a bending power of 1.5 to 5.5 Tm. The RPC detector consists of about 3700 gas volumes with a total surface area of more than 4000 m2. This paper reports on the performance of the RPC detector and L1 muon barrel trigger using 60.8 fb-1 of proton-proton collision data recorded by the ATLAS experiment in 2018 at a centre-of-mass energy of 13 TeV. Detector and trigger performance are studied using Z boson decays into a muon pair. Measurements of the RPC detector response, efficiency, and time resolution are reported. Measurements of the L1 muon barrel trigger efficiencies and rates are presented, along with measurements of the properties of the selected sample of muon candidates. Measurements of the RPC currents, counting rates and mean avalanche charge are performed using zero-bias collisions. Finally, RPC detector response and efficiency are studied at different high voltage and front-end discriminator threshold settings in order to extrapolate detector response to the higher luminosity expected for the High Luminosity LHC.

47 OTHER INSTRUMENTATION↗

Fundamental problems in astroparticle physics and cosmology (Final Technical Report)

In the standard cosmological model, structure forms when gas cools and condenses to the center of dark matter halos. The onset of structure is governed by rapid star formation and subsequent evolution of the first massive stars. One of the endpoints of stellar evolution is the formation of a black hole. We showed that all black hole merger events must occur after the universe is about 85 million years old. This prediction is important because it means that if a future experiment makes a detection of a black hole merger event at an earlier time then our understanding of cosmology and the onset of structure formation is not fully developed. In addition, we explored dark matter models that have either self-interactions or experience decays. In the first case, self-interactions may lead to the formation of a thick disk that can be co-planar to the Galactic disc due to correlations in angular momentum between dark matter and baryons that are predicted by tidal torque theory. We showed that for heavy dark matter particles, either the self interaction may not be strong enough to solve the small scale structure motivation or a dark disc cannot be present in the Milky Way. In the second-case, we showed that if dark matter experiences decays into two particles, one of which behaves like radiation, then it is possible to relieve the tension that exists between measurements of the local expansion rate. Finally, we developed methods on how to distinguish gamma-ray excesses from promising dark matter targets as compared to conventional astrophysical sources. This is an important toolset that is applicable to any suspected dark matter source.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Effects of 18 O Exchange on Neutron Emission Rates of Aging 238 PuO 2 LWRHUs

The Lightweight Radioisotope Heater Unit (LWRHU) provides about 1 Watt of thermal power to critical electrical and mechanical systems in the extreme temperatures of space, maintaining the operating temperature of the spacecraft’s scientific and general operating equipment. Los Alamos National Laboratory (LANL) designed and tested the LWRHU in the 1970s through early 1980s. The first production campaign at LANL was in the early 1980s in support of the Galileo mission in which over 100 LWRHUs were manufactured. In the mid-1990s, almost 200 LWRHUs were manufactured in support of the Cassini mission. After the primary Cassini manufacturing campaign, the Department of Energy (DOE) approved the fabrication of more than 10 additional LWRHUs as spares in 1998. The LWRHU assembly contains the following components: a fuel pellet, a vented capsule, a pyrolytic graphite insulator, and a fine-weave pierced fabric (FWPF) graphite aeroshell. The fuel pellet is a hot-pressed 238 PuO 2 cylindrical pellet that is sintered to create a ceramic pellet. The pellet is encapsulated in a platinum-rhodium encapsulation. The welded fueled clad is placed inside a pyrolytic graphite thermal insulation to protect the fuel from the heat produced in reentry events. The exterior layer of the LWRHU assembly is the FWPF aeroshell. Before sintering, PuO 2 granules are heated in a furnace at temperatures greater than or equal to 700°C under an enriched 16 O atmosphere in order to reduce trace quantities of 18 O. Because 18 O undergoes an (α,n) reaction, 18 O needs to be removed as much as possible to meet radiation emission requirements set by the Jet Propulsion Laboratory (JPL) and the National Aeronautics and Space Administration (NASA), as well as other agencies. The relative abundances of the oxygen isotopes are indicated by neutron emission rate (NER) measurements. LWRHUs are vented with a sintered platinum frit vent (George 1986). During extraterrestrial operation, the vent in the cladding allows helium from the decay of plutonium to escape and relieves pressure from the system while preventing the solids from escaping (Rinehart 1996, Tate 1982 & 1985). This vent is protected during manufacture by a platinum-30 rhodium cover. The capsule vent is activated by milling a 0.025-inch diameter hole through the protective cover to a nominal depth of 0.015 inches, generally immediately before the LWRHU is loaded into the aeroshell (George 1986). Prior to long-term storage, LWRHUs are vented and thus potentially allow infiltration of 18 O from the ambient atmosphere. Although NER decreases with age due to the reduction in emitted alpha particles, it might be expected that NER reduction is mitigated by the exchange of 18 O. However, this is not necessarily the case and no trend was observed relating NER to age other than the natural decay of 238 Pu (Mulford 2021). The most probable and dominant factor for determining specific NER was manufacturing discrepancies between individual units. It is important to understand the lack of observed 16 O- 18 O exchange and to compare LWRHU pellets as much as possible.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Singularities in the gravitational capture of dark matter through long-range interactions

Here, we re-examine the gravitational capture of dark matter (DM) through long-range interactions. We demonstrate that neglecting the thermal motion of target particles, which is often a good approximation for short-range capture, results in parametrically inaccurate results for long-range capture. When the particle mediating the scattering process has a mass that is small in comparison to the momentum transfer in scattering events, correctly incorporating the thermal motion of target particles results in a quadratic, rather than logarithmic, sensitivity to the mediator mass, which substantially enhances the capture rate. We quantitatively assess the impact of this finite temperature effect on the captured DM population in the Sun as a function of mediator mass. We find that capture of DM through light dark photons, as in e.g. mirror DM, can be powerfully enhanced, with self-capture attaining a geometric limit over much of parameter space. For visibly-decaying dark photons, thermal corrections are not large in the Sun, but may be important in understanding long-range DM capture in more massive bodies such as Population III stars. We additionally provide the first calculation of the long-range DM self-evaporation rate.

79 ASTRONOMY AND ASTROPHYSICS↗

Modeling the Conformer-Dependent Electronic Absorption Spectra and Photolysis Rates of Methyl Vinyl Ketone Oxide and Methacrolein Oxide

Criegee intermediates are important atmospheric oxidants, formed via the reaction of ozone with volatile alkenes emitted into the troposphere. Small Criegee intermediates (e.g., CH 2 OO and CH 3 CHOO) are highly reactive, and their removal via unimolecular decay or bimolecular chemistry dominates their atmospheric lifetimes. As the molecular complexity of Criegee intermediates increases, their electronic absorption spectra show a bathochromic shift within the solar spectrum relevant to the troposphere. In such cases, solar photolysis may become a competitive contributor to their atmospheric removal. In this article, we report the conformer-dependent simulated electronic absorption spectra of two four-carbon-centered Criegee intermediates, methyl vinyl ketone oxide (MVK-oxide) and methacrolein oxide (MACR-oxide). Both MVK-oxide and MACR-oxide contain four low-energy conformers, which are convoluted in the experimentally measured spectra. Here, we deconvolute each conformer and estimate contributions from each of the four conformers to the experimentally measured spectra. We also estimate the photolysis rates and predict that solar photolysis should be a more competitive removal process for MVK-oxide and MACR-oxide (cf. CH 2 OO and CH 3 CHOO).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Constraints on Higgs boson properties using $WW^*(→eνμν)jj$ production in 36.1fb -1 of $\sqrt{s}$ = 13 TeV pp collisions with the ATLAS detector

This article presents the results of two studies of Higgs boson properties using the WW * (→eνμν)jj final state, based on a dataset corresponding to 36.1fb -1 of $\sqrt{s}$ =13 TeV proton–proton collisions recorded by the ATLAS experiment at the Large Hadron Collider. The first study targets Higgs boson production via gluon–gluon fusion and constrains the CP properties of the effective Higgs–gluon interaction. Using angular distributions and the overall rate, a value of tan(α)=0.0±0.4(stat.)±0.3(syst.) is obtained for the tangent of the mixing angle for CP-even and CP-odd contributions. The second study exploits the vector-boson fusion production mechanism to probe the Higgs boson couplings to longitudinally and transversely polarised W and Z bosons in both the production and the decay of the Higgs boson; these couplings have not been directly constrained previously. The polarisation-dependent coupling-strength scale factors are defined as the ratios of the measured polarisation-dependent coupling strengths to those predicted by the Standard Model, and are determined using rate and kinematic information to be a L =0.91$^{+0.10}_{-0.18}$(stat.)$^{+0.09}_{-0.17}$(syst.) and a T =1.2±0.4(stat.)$^{+0.2}_{-0.3}$(syst.). These coupling strengths are translated into pseudo-observables, resulting in κ VV =0.91$^{+0.10}_{-0.18}$(stat.)$^{+0.09}_{-0.17}$(syst.) and ϵ VV =0.13$^{+0.28}_{-0.20}$ (stat.)$^{+0.08}_{-0.10}$(syst.). All results are consistent with the Standard Model predictions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Measurement of the Higgs boson production via vector boson fusion and its decay into bottom quarks in proton-proton collisions at $\sqrt{s}$ = 13 TeV

A measurement of the Higgs boson (H) production via vector boson fusion (VBF) and its decay into a bottom quark-antiquark pair ($\mathrm{b\bar{b}}$) is presented using proton-proton collision data recorded by the CMS experiment at $\sqrt{s}$ = 13 TeV and corresponding to an integrated luminosity of 90.8 fb$^{-1}$. Treating the gluon-gluon fusion process as a background and constraining its rate to the value expected in the standard model (SM) within uncertainties, the signal strength of the VBF process, defined as the ratio of the observed signal rate to that predicted by the SM, is measured to be $\mu^\text{qqH}_\mathrm{Hb\bar{b}}$ = 1.01$^{+0.55}_{-0.46}$. The VBF signal is observed with a significance of 2.4 standard deviations relative to the background prediction, while the expected significance is 2.7 standard deviations. Considering inclusive Higgs boson production and decay into bottom quarks, the signal strength is measured to be $\mu^\text{incl.}_\mathrm{Hb\bar{b}}$ = 0.99$^{+0.48}_{-0.41}$, corresponding to an observed (expected) significance of 2.6 (2.9) standard deviations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Ab initio calculation of the β-decay spectrum of 6 He

Here, we calculate the β spectrum in the decay of 6 He using quantum Monte Carlo methods with nuclear interactions derived from chiral effective field theory and consistent weak vector and axial currents. We work at second order in the multipole expansion, retaining terms suppressed by O(q 2 /m$^{2}_{π}$), where q denotes low-energy scales such as the reaction’s Q value or the electron energy, and m π is the pion mass. We go beyond the impulse approximation by including the effects of two-body vector and axial currents. We estimate the theoretical error on the spectrum by using four potential models in the Norfolk family of local two- and three-nucleon interactions, which have different cutoffs, fit two-nucleon data up to different energies, and use different observables to determine the couplings in the three-body force. We find the theoretical uncertainty on the β spectrum, normalized by the total rate, to be well below the permille level, and to receive contributions of comparable size from first- and second-order corrections in the multipole expansion. We consider corrections to the β decay spectrum induced by beyond-standard-model charged-current interactions in the standard model effective field theory, with and without sterile neutrinos, and discuss the sensitivity of the next generation of experiments to these interactions.

6 ≤ A ≤ 19↗

Enabling stable and high-rate cycling of a Ni-rich layered oxide cathode for lithium-ion batteries by modification with an artificial Li⁺-conducting cathode-electrolyte interphase

Ni-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathodes are investigated to realize high energy density Li ion batteries for long life electric vehicle applications. However, capacity decay and thermal instability due to cathode-electrolyte interfacial degradation remain challenges that require sophisticated surface stabilization methods to address. Here, we propose a strategy, for the first time, to form an artificial Li + -conducting cathode-electrolyte interphase (ALCEI) on the NCM811 cathode surface using a nucleophilic reaction between polysulfides and vinylene carbonate (VC). Furthemore, the as-formed ALCEI layer simultaneously protects the NCM particles from electrolyte corrosion and facilitates Li + ion transport, thus enabling stable and high rate cycling of NCM811. As a result, the ALCEI-modified NCM811 cathode exhibits a high capacity (211.6 mA h g -1 at 0.1C), notable rate capability (134 mA h g -1 at 10C), and superior cycle stability (94.2% over 200 cycles at 1C). These results underscore the use of interfacial engineering in high voltage cathode material development and provide a feasible strategy for stabilizing Ni-rich cathode interfaces in practical Li ion battery applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Assessment of Thin Plastic Scintillation Detectors for Beta-Particle Measurements at the Advanced Test Reactor Critical Facility

The Fission Wire Measurement System is a custom measurement system designed in the 1960s to measure the beta-particle activity of irradiated uranium-aluminum fission wires. This measurement is conducted to determine the fission rate profile of the Advanced Reactor Test Critical facility. The Advanced Test Reactor Critical facility is an open-pool, low-power test reactor used to qualify experiment configurations and verify core models prior to full-power experiment irradiations in the Advanced Test Reactor. Power distribution measurements in ATR-C use uranium-aluminum wires that are distributed throughout the core to validate simulation and modeling results. These measurements require from 340 to 1500 wires to be irradiated and measured within a 12-hour window. The system consists of 4 measurement channels and one reference channel, each with a 2-pi proportional gas flow detector and the measurement channels each have an automated sample changer. The gas flow detectors are of a custom design for this detector system that use methane gas with a large anode wire compared to modern proportional counters. These detectors, which are nearly 60 years old are irreplaceable. The measurements from these gas detectors are affected by the gas flow rate, atmospheric and line pressure, and are very sensitive to the applied high voltage. Recent improvements have been made to the control and data acquisition system, but the detectors have remained the same. The nature of the measurement of the fission product decay activity is such that the energy spectrum of the signal is changing with time. Thin, 250-um thick, plastic scintillators were commercially obtained as a potential replacement for the gas flow detectors. The original calibration of the uranium-aluminum fission wires was conducted in 1965 using a series of irradiations of gold foils and the wires in a well-characterized thermal neutron field. These measurements provided a time-dependent fission rate conversion factor from the gold foil data to calibrate the fission wires based on the response from the 2-pi proportional gas detectors. Transitioning to the new detectors requires qualification and testing. The sensitivity of the scintillators to changes in the energy spectrum of the fission wires and translation of the calibration factor have been completed. These measurements indicated that the sensitivity of the scintillators over time changes at a different rate than the sensitivity of the gas flow detectors. However, the inverse activity of measurements of both detector types is linear with time. Initial results indicate that the scintillator detectors will be a sufficient replacement for the gas detectors with minor adjustments to the fission rate conversion factor. Replacement of the detectors will improve the fission wire measurements and provide a more stable and reliable measurement system.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Electron capture of superheavy nuclei with realistic lepton wave functions

The superheavy nuclei push the periodic table of the elements and the chart of the nuclides to their limits, providing a unique laboratory for studies of the electron-nucleus interactions. The most important weak decay mode in known superheavy nuclei is electron capture (EC). In the standard calculations of EC, the lepton wave functions are usually considered in the lowest-order approximation. In this work, we investigate the sensitivity of EC rates on the choice of the electron wave functions by (i) assuming the single-particle approximation for the electron wave functions, and (ii) carrying out Dirac-Hartree-Fock (DHF) calculations. The nuclear response is generated based on the state-of-the-art quasiparticle random phase approximation employing relativistic nuclear energy density functional theory. Here, we show that using the improved lepton wave functions reduces the EC rates up to 40% in the superheavy nucleus oganesson (𝑍=118). Interestingly, because of screening effects, the difference between the EC rates obtained with the DHF and single-particle calculations is fairly small.

Atomic orbital↗

Unveiling the origins of work-hardening enhancement and mechanical instability in laser shock peened titanium

Laser shock-peening (LSP) produces complex gradients in microstructures and residual stresses, which enables fabrication of metallic engineering components with superior mechanical properties. In this work, we use non-destructive and spatially resolved high-energy X-ray diffraction (HE-XRD) to investigate the influences of LSP on microstructure, surface topography, and residual stress for high purity titanium plates. LSP is found to produce large compressive in-plane residual stresses near the peened surface which monotonically decay to zero about 2.5 mm below the surface. These properties were also tracked during in-situ tensile loading, allowing stress partitioning and work-hardening rates to be measured as a function of depth. The surface region is found to have the highest work-hardening rate and remain mechanically stable up to sample failure. In addition, a crystal rigid rotation along a transversal axis of about 27 & nbsp; was observed at large applied strain near the surface region, which is attributed to the formation of denser dispersed shear bands. Furthermore, a sudden drop in tensile stress was observed at a depth of similar to 160 mu m from the LSP surface, indicating the formation of a localized mechanical instability zone (LMIZ). The origin of this LMIZ could be attributed to the increase in shear stress induced by a load transfer from LSP surface due to the formation of denser dispersed shear bands. These observations indicate a localized transition in deformation behavior has occurred from dispersed shear banding to LMIZ and homogeneous deformation.

36 MATERIALS SCIENCE↗

Structure and function of a flavin-dependent S-monooxygenase from garlic ( Allium sativum )

Allicin is a component of the characteristic smell and flavor of garlic ( Allium sativum ). A flavin-containing monooxygenase (FMO) produced by A. sativum (AsFMO) was previously proposed to oxidize S-allyl- L -cysteine (SAC) to alliin, an allicin precursor. In this paper, we present a kinetic and structural characterization of AsFMO that suggests a possible contradiction to this proposal. Results of steady-state kinetic analyses revealed that AsFMO exhibited negligible activity with SAC; however, the enzyme was highly active with L -cysteine, N-acetyl- L -cysteine, and allyl mercaptan. We found that allyl mercaptan with NADPH was the preferred substrate-cofactor combination. Rapid-reaction kinetic analyses showed that NADPH binds tightly ($K_D$ of ~2 μM) to AsFMO and that the hydride transfer occurs with pro-R stereospecificity. We detected the formation of a long-wavelength band when AsFMO was reduced by NADPH, probably representing the formation of a charge-transfer complex. In the absence of substrate, the reduced enzyme, in complex with NADP + , reacted with oxygen and formed an intermediate with a spectrum characteristic of C4a-hydroperoxyflavin, which decays several orders of magnitude more slowly than the $k$ cat . The presence of substrate enhanced C4a-hydroperoxyflavin formation and, upon hydroxylation, oxidation occurred with a rate constant similar to the $k$ cat . The structure of AsFMO complexed with FAD at 2.08-Å resolution features two domains for binding of FAD and NADPH, representative of class B flavin monooxygenases. These biochemical and structural results are consistent with AsFMO being an S-monooxygenase involved in allicin biosynthesis through direct formation of sulfenic acid and not SAC oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Findings during Incorporation of the Federal Guidance Report No. 15 External Dose Coefficients into the RESRAD Family of Codes

Argonne National Laboratory was tasked by the U.S. Department of Energy (DOE) to incorporate the recently published Federal Guidance Report No. 15 (FGR 15) (EPA 2019) external dose rate coefficients into the database of the RESRAD family of codes. FGR 15 is one of two publications that contain age-specific external effective dose rate coefficients that are based on the International Commission on Radiological Protection (ICRP) Publication 103 (ICRP-103) methodology (ICRP 2007) and the ICRP-107 (ICRP 2008) nuclear decay data; ICRP-144 (ICRP 2020) is the other publication.

61 RADIATION PROTECTION AND DOSIMETRY↗

Initial Testing of Alkaline Earth Metal Ion Absorption on Crystalline Silicotitanate - 20440

The Tank Closure Cesium Removal process at the Savannah River Site (SRS) has processed aqueous tank waste using the inorganic ion exchange media IONSIV{sup TM} R9120-Ba (which is also known as Crystalline Silicotitanate (CST)). Salt-cake in Tank 10H at SRS was dissolved and processed through filters and ion exchange columns. The primary purpose of the process is to remove Cs-137 from the aqueous waste so that it can be disposed as low level waste. It is known that this inorganic media also absorbs strontium from solution, and that strontium competes with cesium ions for absorption sites. The strontium ion is actually more strongly absorbed than the cesium ion from typical tank waste. However, strontium is typically present in low concentrations so does not normally cause a significant impact. Strontium is present as both non-radioactive isotopes and the radioactive Sr-90 isotope; with the non-radioactive isotopes being much more abundant. Although the total strontium solubility is usually much lower than cesium, some tank waste compositions can have a high enough soluble strontium concentration to decrease the cesium absorption. Relatedly, some testing at SRS suggested that another alkaline earth metal, calcium, may also absorb onto CST and may decrease cesium absorption. Barium is also an important species in treatment of tank waste, but is also usually present at low concentrations. However, after the Cs-137 is absorbed onto CST, it emits a beta particle and converts to Ba-137m, which then decays to non-radioactive Ba-137 by emission of a gamma ray. If the Ba-137m were to desorb quickly, it could impact the dose rate in down-stream equipment. In order to understand the impact of these alkaline earth metals on CST, SRNL performed testing using simulants of SRS tank waste that contain soluble barium, strontium, and calcium. Testing examined both removal of the alkaline earth metals and their impact on removal of cesium. Testing involved first developing realistic waste simulant formulations and dissolving the alkaline earth metals to high enough concentrations to potentially impact the Cs absorption. Once the formulations were developed and prepared, computer modeling was used to calculate the expected Cs absorption behavior to determine if the alkaline earth metals impact the performance. Measurements of the alkaline earth metals absorption by the media is also important for disposition of spent media because of the added radionuclide inventory from the Sr-90. These initial tests are examining the general impact and will be used to determine if further testing or measurements are needed. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗