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At least 613 records · Page 34

The solubility of titanite in silicate melt determined from growth and dissolution experiments

The solubility of titanite (CaTiSiO 5 ) in Si-rich melts was measured experimentally through growth experiments at 800–1000 °C, 0.5–1.0 GPa, log fO 2 ~ CCO–0.8, t = 72–168 h, and H 2 O = 0 to 4 wt.%, and in dissolution experiments at 925–1300 °C, 0.8 GPa, t = 18–118 h, and H 2 O = 1–10 wt.% in a piston-cylinder apparatus. Run product glasses in growth experiments were homogeneous, and iron loss suppressed ilmenite crystallization. Saturation concentrations in dissolution experiments were estimated by fitting measured diffusion profiles. Titanite solubility increases with increasing temperature and melt composition parameter \(M = {\text{ molar }}\left( {{\text{Na }} + {\text{ K }} + {\text{ 2Ca}}} \right)/\left( {{\text{Al }} \times {\text{ Si}}} \right)\) . Multiple linear regression of glass composition data from growth and dissolution experiments ( n = 29) plus 39 experiments from the LEPR database (Hirschmann et al. 2008 ) yielded the titanite solubility equation (adj. r 2 = 0.95): \(\left( {TiO_{2} } \right)^{melt} \left( {wt.\% } \right) = 0.978 \times M + 0.0048 \times T\left( K \right){-}5.90\) . This model correctly predicted undersaturation in 95% of 2344 experiments from the LEPR database that did not have titanite or rutile. Application to natural rocks yields saturation temperatures that are similar to independent temperature estimates. Finally, this equation should be useful for constraining the temperatures of titanite-saturated melts, for determining whether titanite saturation in magmatic source regions is likely, and for determining when titanite can crystallize and begin to exert an influence on melt geochemistry.

58 GEOSCIENCES↗

Effect of dilute Rh on oxygen dissociation, spillover, and the oxidation of Cu across many orders of magnitude pressure

Knowledge of how trace amounts of more reactive metals influence the oxidation rate and mechanism of Cu surfaces is essential for developing strategies to optimize the performance of Cu-based catalysts. We find that the addition of 1% Rh to Cu(111) increases the initial O 2 dissociation rate by approximately 9-fold. CO poisoning experiments reveal that single Rh atoms activate O 2 and facilitate the spillover of atomic oxygen to Cu sites. Scanning tunneling microscopy (STM) and in situ X-ray photoelectron spectroscopy (XPS) support this mechanism, showing enhanced surface oxygen near Rh atoms. Here, a density functional theory (DFT)-based model demonstrates that Rh binds the O 2 precursor 0.15 eV more strongly than Cu(111) and lowers the O 2 dissociation barrier by 0.02 eV. Both single-crystal and nanoparticle experiments show that at low oxygen pressures, Rh enhances Cu oxidation, whereas at higher pressures, it inhibits deeper oxidation, as evidenced by in situ ultraviolet-visible (UV-vis) spectra.

36 MATERIALS SCIENCE↗

Axions beyond Gen 2

The QCD (Quantum ChromoDynamics) axion emerged as one of the best-motivated dark matter candidates. In 2018, the Axion Dark Matter eXperiment (ADMX), one of the U.S. Department of Energy’s “Gen 2” flagship dark-matter projects, demonstrated first sensitivity to the highly plausible “DFSZ” dark matter axion couplings over a small frequency range. We anticipate this development marks the first step in constructing yet more powerful experiments that can explore large swaths of the axion parameter space at high sensitivity and result in a discovery. But, realizing this requires advances in both our understanding of the theory and experiment design. Between 25 January and 27 January 2021, the “Axions Beyond Gen 2 Workshop” was held, where selected members of the community discussed our broad understanding of the QCD axion and charted a course for future experiments having sensitivity and mass reach well beyond the current “Gen 2” experiments. These proceedings are summaries of the topics presented and discussed.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Electroenzymatic Nitrogen Fixation Using a MoFe Protein System Immobilized in an Organic Redox Polymer

Abstract We report an organic redox‐polymer‐based electroenzymatic nitrogen fixation system using a metal‐free redox polymer, namely neutral‐red‐modified poly(glycidyl methacrylate‐ co ‐methylmethacrylate‐ co‐ poly(ethyleneglycol)methacrylate) with a low redox potential of −0.58 V vs. SCE. The stable and efficient electric wiring of nitrogenase within the redox polymer matrix enables mediated bioelectrocatalysis of N 3 − , NO 2 − and N 2 to NH 3 catalyzed by the MoFe protein via the polymer‐bound redox moieties distributed in the polymer matrix in the absence of the Fe protein. Bulk bioelectrosynthetic experiments produced 209±30 nmol NH 3 nmol MoFe −1 h −1 from N 2 reduction. 15 N 2 labeling experiments and NMR analysis were performed to confirm biosynthetic N 2 reduction to NH 3 .

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Sequential spectral line analysis for accurate density and temperature diagnosis of laboratory opacity measurements

The accuracy of iron opacity calculated in stellar interiors has been questioned since the discovery of the “solar problem” and the discrepancies between the measured and modeled iron opacity reported in 2015. Experimental opacity benchmarks require accurate temperature and density measurements, which were inferred by analyzing tracer magnesium spectra in those experiments. Could the observed discrepancy be explained by insufficient accuracy in the inferred temperature, density, and their uncertainties? Previous analyses may have yielded biased results due to three limitations: (1) simultaneous multi-line fitting, (2) approximations in line-shape models, and (3) exclusion of certain spectral lines due to insufficient background characterization. Notably, the first issue is a common concern for many inversion methods, including Bayesian inferences. We present a refined analysis method that overcomes these limitations, applied to three categories of iron opacity experiments (Anchor 1, 2, and 3). In particular, the sequential fitting method yields unbiased results with more realistic uncertainties by accounting for line inconsistencies in the parameter uncertainties. The average electron temperature and density values are 162 ± 6 eV and (7.0 ± 1.9) × 10 21 cm −3 for six Anchor 1 experiments, 189 ± 7 eV and (3.4 ± 0.3) × 10 22 cm −3 for 21 Anchor 2 experiments, and 201 ± 6 eV and (4.8 ± 1.1) × 10 22 cm −3 for nine Anchor 3 experiments. These results show ∼4% temperature and ∼20% density reproducibility over a decade, which also aligns with the inferred parameter uncertainties. In conclusion, the resulting temperature and density uncertainties lead to a quasi-continuum iron opacity variation of ±4%–7% for wavelengths below 9.5 Å, which is insufficient to explain the significant model-data discrepancies reported in 2015.

Absorption spectroscopy↗

Spin dynamics in linear magnetoelectric material Mn 3 Ta 2 O 8

We performed inelastic neutron scattering experiments on single crystal samples of a linear magnetoelectric material Mn 3 Ta 2 O 8 , which exhibits a collinear antiferromagnetic order, to reveal the spin dynamics. Numerous modes observed in the neutron spectra were reasonably reproduced by linear spin-wave theory on the basis of the spin Hamiltonian including eight Heisenberg interactions and an easy-plane type single-ion anisotropy. In conclusion, the presence of strong frustration was found in the identified spin Hamiltonian.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Design, Analysis, and Experimental Testing of Hydrogen Lean Direct Injection Nozzles at Elevated Pressure

Abstract There are many challenges of commissioning a hydrogen combustor into future gas turbine engines; especially regarding achieving emissions goals. Previously, Escudero et al. and Tran et al. conducted a study to adapt the liquid fuel Lean Direct Injection (LDI) concept from Jet-A to gaseous natural gas-hydrogen blends and pure hydrogen [1], [2]. Experimental data was collected at atmospheric conditions using a Box Behnken design of experiments. The design of experiments suggested that biasing the air split in favor of the inner air circuit and increasing the swirl strength of this inner air passage resulted in improved NOx emissions, while the inverse was true for stability, which was quantified by studying the lean blowoff point (LBO) [1], [2]. The trends revealed by the original experiment [1], [2] provided a design direction for further iterations of the experimental hardware. The study presented herein describes the further investigation of such LDI injectors through experimental methods and computational fluid dynamic (CFD) simulations at atmospheric conditions, which were used to identify potential flow behaviors driving enhanced emissions performance. Further evaluation of select injectors from both studies was then conducted at elevated pressures up to 6 atmospheres. The results from both experiments are presented in this study, which include flame observations, emissions measurements, and operational challenges. NOx emissions results are reported on a volume basis in ppmvd corrected to 15% O2 and corrected for fuel. A predictive model for relating NOx emissions to test conditions at atmospheric conditions show high significance to adiabatic flame temperature while little to no significance to fuel composition for the best performing configurations. The results illustrate the connection between atmospheric testing and testing elevated pressures. The design direction indicated by the initial tests and CFD results in promising configurations for implementation into a Multi-point LDI array.

08 HYDROGEN↗

Wettability variation and its impact on CO 2 storage capacity at the Wyoming CarbonSAFE storage hub: An experimental approach

Meeting global and national net zero carbon emission targets will require geologic carbon disposal. The U.S. Department of Energy (DOE) has accordingly funded significant research in this area, including the Wyoming CarbonSAFE project at Dry Fork Station (DFS) in Campbell County, Wyoming. This work studied wettability on micro- and macro-scales, CO 2 storage potential, and the correlation between the two to support the Wyoming CarbonSAFE project’s subsurface assessment. During the study, a target formation’s wettability was found to affect how much CO 2 can be stored in a given formation. Here, in this study, representative rock samples were selected from the target storage formations— Lakota, Hulett, and Minnelusa—based on the heterogeneity of the lithology, permeability, and porosity of the respective formations. The rock samples are all fine-grained sandstone with variable cementation and bedding structure, including different scales of laminated bedding. The porosity and permeability vary within the range of 9.0–14.3% and 0.1–28.9 mD, respectively. These rock samples were prepared for the micro-scale wettability (contact angle measurement), macro-scale wettability (wettability index derived from unsteady-state flow characterization for the core plugs), and CO 2 storage evaluation. The macro-scale experiments suggested that wettability appeared to dominate the CO 2 storage potential performance during the drainage process, where less water-wet behavior promoted higher CO 2 storage potential. The micro-scale wettability tests showed that the rock samples at the studied reservoir conditions behaved water-wet and became more water-wet as pressure increased. This kind of wettability change discourages further CO 2 storage potential yet benefits the CO 2 residual trapping as the CO 2 injection proceeds for the studied area. The results allow the recommendation of the best reservoir candidate for storage based on wettability that affects CO 2 storage. The work presented in this study provides valuable insights into wettability’s effect on the CO 2 storage capacity and wettability’s importance when identifying the optimal CO 2 storage formation to meet the project’s goals.

58 GEOSCIENCES↗

Nickel promotes selective ethylene epoxidation on silver

Over the last 80 years, chlorine (Cl) has been the primary promoter of the ethylene epoxidation reaction valued at ~40 billion USD per year, providing a ~25% selectivity increase over unpromoted silver (Ag) (~55%). Promoters such as cesium, rhenium, and molybdenum each add a few percent of selectivity enhancements to achieve 90% overall, but their codependence on Cl makes optimizing and understanding their function complex. Here, we took a theory-guided, single-atom alloy approach to identify nickel (Ni) as a dopant in Ag that can facilitate selective oxidation by activating molecular oxygen (O 2 ) without binding oxygen (O) too strongly. Surface science experiments confirmed the facile adsorption/desorption of O 2 on NiAg, as well as demonstrating that Ni serves to stabilize unselective nucleophilic oxygen. Supported Ag catalyst studies revealed that the addition of Ni in a 1:200 Ni to Ag atomic ratio provides a ~25% selectivity increase without the need for Cl co-flow and acts cooperatively with Cl, resulting in a further 10% initial increase in selectivity.

36 MATERIALS SCIENCE↗

Monitoring SARS-CoV-2 in wastewater

The detection of SARS-CoV-2 cases throughout the pandemic has been based on individual testing, which is subject to inaccuracies in what is actually occurring within the local population. Wastewater biosurveillance has been used around the world to detect the presence of drugs, viruses, and other chemicals present in a population. Fecal shedding of SARS-CoV-2 implies that wastewater can be analyzed in order to detect varying levels of the virus within a given community. This analysis can show the fluctuation of SARS-CoV-2 at a population level over time. In this experiment, the amount of SARS-CoV-2 in the wastewater sample was compared to the amount of Pepper Mild Mottle Virus (PMMoV) detected in the same sample. PMMoV is present consistently in human fecal matter, and can be used to normalize the amount of SARS-CoV-2 detected in wastewater.

59 BASIC BIOLOGICAL SCIENCES↗

Gapless surface electronic structure of $1T–$$\mathrm{TiSe_2}$ in the distorted phase

Here, low temperature, high resolution angle resolved photoemission experiments performed on bulk $1T–$$\mathrm{TiSe_2}$ samples display conspicuous band folding as the only prominent signature of the periodic lattice distortion. The presence of a bulk electronic gap supporting a charge density wave phase is not confirmed in light of the new data. These observations cast serious doubts on the common belief of an electronic instability as the likely origin for the observed structural transition in $\mathrm{TiSe_2}$.

36 MATERIALS SCIENCE↗

Electron recombination of rotationally cold D 2 H + ions

Dissociative recombination (DR) of electrons with small molecular ions is a fundamental process for the physics and chemistry of the interstellar medium and planetary atmospheres. In previous DR studies, detailed analysis of the experimental rate coefficients has been hindered by the difficulty of preparing the ions in well-defined quantum states. For polyatomic ions in particular, truly state-selective measurements have been elusive, allowing only qualitative benchmarks of theory. Here, we present DR studies of the deuterated triatomic hydrogen ion D 2 H + , where the molecular ions were stored for up to 1000 seconds inside the Cryogenic Storage Ring (CSR) prior to the DR measurements. Our experiments with rotationally cold D 2 H + ions allow for detailed comparison to state-of-the-art theoretical calculations. We obtain very good agreement between experiment and theory even in the important collision energy range from 1 meV to 0.5 eV, where a multitude of Rydberg resonances reveal their imprint on the rate coefficient.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Pulsed-Neutron Die-Away Response of H 2 O Targets to a D-T Generator Pulse

Pulsed-neutron die-away (PNDA) experiments were completed at Lawrence Livermore National Laboratory (LLNL). The goal of these experiments was to provide a benchmark to validate thermal neutron scattering laws of H 2 O. The experiment was conducted with a deuterium-tritium (D-T) neutron generator producing pulses of 14.1 MeV neutrons that impinged on a moderating target. The neutrons scattered and thermalized within the target and were counted as a function of time using Helium-3 ( 3 He) detectors that surrounded the target. These data provide a time-decay profile of the neutron population from which the time eigenvalue of the experiment is calculated. The time eigenvalue quantity α represents the integral parameter of interest. This report describes the measurements for H 2 O targets. The measurements were conducted over several days beginning on October 23rd, 2023. All measurements were completed at the low-scatter facility at LLNL. The evaluation identifier is FUND-LLNL-DT-H2O-PNDA-001.

3He Detectors↗

Why are Lead Iodide‐Based Perovskite Precursor Inks Yellow?

A challenge faced by metal halide perovskite (MHP) photovoltaics is scaling up solution deposition processes to realize rapid and inexpensive manufacturing. The challenge lies in completely understanding and controlling solution speciation, nucleation, and self-assembly of iodoplumbate complexes during solvent evaporation as the liquid transforms into gels and solids. An accurate description of solution species, at all points in the transformation, is a prerequisite to design robust and reliable processes. Here, in this study, the common assumption that initial monoplumbate solution species typically invoked (e.g., [PbI 6 ] 4− ) are certainly not the origin of optical absorbance at >400 nm wavelengths is disproved, as are many large particles of common “intermediate” iodoplumbate phases with face- or edge-sharing connectivity. Instead, a new perspective is offered, involving (partially) corner-sharing iodo(poly)plumbates (>1 Pb 2+ per complex) that experience highly dynamic chemical environments. It is outlined how the MHP field would benefit by elucidating these phenomena. Future work is required to determine the size and kinetic behavior of polyplumbate species, and contextualize these findings in relation to broader trends in materials chemistry beyond MHPs. Ultimately, a complete explanation for the solution speciation, optical absorbance signatures, and the color of MHP precursor inks remains an open challenge to the community.

14 SOLAR ENERGY↗

Modeling and simulation of gas separations with spiral–wound membranes

Models for gas separations with spiral–wound membranes are developed and found to exhibit good agreement with experiments performed on N 2 /O 2 mixtures. The two–dimensional (2D) model can be accurately approximated by a one–dimensional (1D) surrogate model when the spacer widths are chosen to make the channel pressure drops small. Subsequently, the separation of propane/propylene mixtures from the recycle purge stream of a polypropylene reactor is investigated. Assuming ideal gas is found to lead to significant overestimations in membrane stage cuts (sometimes more than 10%), an extent comparable to that associated with extrapolating constant olefin permeance from a low–pressure condition. While olefin permeance can change significantly with pressure, using a constant–permeance formulation can result in a small (< 2.5%) underprediction in stage cut if the value for the permeance is taken from the feed condition. Finally, membrane properties and costs necessary for a viable separation process are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Magnetic nanoparticle‐induced sorbent regeneration for direct air capture

Direct air capture (DAC) is a promising technology for decarbonization through the removal of CO 2 from the atmosphere. In many DAC processes, the regeneration energy used to restore the capture capacity of sorbents accounts for a significant fraction of the energy required by the whole process. Here we report an effective and scalable sorbent regeneration method for liquid DAC solvents based on magnetic nanoparticles (MNPs) heating with AC magnetic fields. MNPs can be directly heated to provide uniform and rapid volumetric heating, as we demonstrate by promoting the release of captured CO 2 from an aqueous solution of potassium sarcosinate. Our results showed that 90% of the solvent can be regenerated within 7.5 min of heating through proposed technique. The MNPs and solvent are found to be stable during the regeneration process and the MNPs showed long-term stability in the CO 2 -saturated solvent. Cyclic experiments showed that the nanoparticles can be reused for multiple cycles without performance deterioration. The process is operated in a noncontact mode through electromagnetic waves, making it an adoptable approach for existing carbon capture systems. The MNPs heating provides an effective regeneration strategy for liquid solvents used in carbon capture processes, in particular for DAC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Search for excited $τ$-leptons and leptoquarks in the final state with $τ$-leptons and jets in pp collisions at $\sqrt{s}$ = 13 TeV with the ATLAS detector

A search is reported for excited $τ$-leptons and leptoquarks in events with two hadronically decaying $τ$-leptons and two or more jets. The search uses proton-proton ($pp$) collision data at $\sqrt{s}$ = 13 TeV recorded by the ATLAS experiment during the Run 2 of the Large Hadron Collider in 2015–2018. The total integrated luminosity is 139 fb -1 . The excited $τ$-lepton is assumed to be produced and to decay via a four-fermion contact interaction into an ordinary $τ$-lepton and a quark-antiquark pair. The leptoquarks are assumed to be produced in pairs via the strong interaction, and each leptoquark is assumed to couple to a charm or lighter quark and a $τ$-lepton. No excess over the background prediction is observed. Excited $τ$-leptons with masses below 2.8 TeV are excluded at 95% CL in scenarios with the contact interaction scale Λ set to 10 TeV. At the extreme limit of model validity where Λ is set equal to the excited $τ$-lepton mass, excited $τ$-leptons with masses below 4.6 TeV are excluded. Leptoquarks with masses below 1.3 TeV are excluded at 95% CL if their branching ratio to a charm quark and a $τ$-lepton equals 1. The analysis does not exploit flavour-tagging in the signal region.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Design of Mini-Plate-1 Irradiation Test for Qualification of High-Density, Low-Enriched U-10Mo Monolithic Fuel

The United States High Performance Research Reactor project is tasked with fuel development and qualification leading to conversion of higher power research and test reactors in the US from high-enriched uranium (HEU) to low-enriched uranium (LEU) fuels. Here, this manuscript identifies the functional and operational design requirements of the first miniature test plate (mini-plate [MP]) irradiation campaign (MP-1) of commercially fabricated LEU U-10Mo monolithic plate-type fuel and is the precursor to a large parametric mini-plate test (MP-2) aimed at producing the data to support regulatory qualification of the LEU U-10Mo monolithic fuel. The manuscript (1) provides a general description of the selected U-10Mo LEU fuel and (2) defines the overall experiment design and functional requirements to accomplish the specific test objective of MP-1, which is to confirm that the commercially manufactured LEU U-10Mo monolithic fuel meets the established requirements of geometric stability, mechanical integrity and stable and predictable behavior. The fuel testing parameters are established by the need to bound performance behavior within the operational envelope of the reactors being converted.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗