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At least 253 records · Page 14

Fischer-Tropsch synthesis: Direct cobalt nitrate reduction of promoted Co/Al 2 O 3 catalysts

Direct reduction of cobalt nitrate versus conventional calcination/reduction treatment was conducted using alumina with identical methodology as previously applied to SiO 2 and TiO 2 . Similar BET surface areas, pore volumes and pore size distributions were obtained for the activated calcined and uncalcined catalysts indicating no significant difference on morphological properties. However, the reducibility slightly increases and Co crystallite size is smaller for activated uncalcined samples. Reduction phenomena were analyzed by TPR-MS and TPR-EXAFS/XANES. Combining these techniques allows an explanation of the complex phenomena occurring during the direct reduction of cobalt nitrate, as both nitrate decomposition and cobalt oxide reduction are involved. Cobalt nitrate species are converted to CoO x intermediates. These species are oxidized by NO X (from nitrate decomposition) to Co 3 O 4 spinel, which is converted to CoO prior to Co 0 formation. Noble metals (Pt, Re, Ru and Ag) improve cobalt oxide reducibility, especially for the final reduction step (i.e., CoO to Co 0 ). The effect of direct nitrate reduction on FT activity was investigated using a 1 L CSTR. Activated unpromoted and Pt-promoted uncalcined catalysts achieved higher initial and steady-state CO conversions in comparison to the corresponding calcined catalysts. The best performance was achieved with direct reduction of uncalcined 0.5%Pt-25%Co/Al 2 O 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Biomass burning aerosols in most climate models are too absorbing

Uncertainty in the representation of biomass burning (BB) aerosol composition and optical properties in climate models contributes to a range in modeled aerosol effects on incoming solar radiation. Depending on the model, the top-of-the-atmosphere BB aerosol effect can range from cooling to warming. By relating aerosol absorption relative to extinction and carbonaceous aerosol composition from 12 observational datasets to nine state-of-the-art Earth system models/chemical transport models, we identify varying degrees of overestimation in BB aerosol absorptivity by these models. Modifications to BB aerosol refractive index, size, and mixing state improve the Community Atmosphere Model version 5 (CAM5) agreement with observations, leading to a global change in BB direct radiative effect of -0.07 W m -2 , and regional changes of -2 W m -2 (Africa) and -0.5 W m -2 (South America/Temperate). Our findings suggest that current modeled BB contributes less to warming than previously thought, largely due to treatments of aerosol mixing state.

54 ENVIRONMENTAL SCIENCES↗

Climate change, malaria and neglected tropical diseases: a scoping review

Abstract To explore the effects of climate change on malaria and 20 neglected tropical diseases (NTDs), and potential effect amelioration through mitigation and adaptation, we searched for papers published from January 2010 to October 2023. We descriptively synthesised extracted data. We analysed numbers of papers meeting our inclusion criteria by country and national disease burden, healthcare access and quality index (HAQI), as well as by climate vulnerability score. From 42 693 retrieved records, 1543 full-text papers were assessed. Of 511 papers meeting the inclusion criteria, 185 studied malaria, 181 dengue and chikungunya and 53 leishmaniasis; other NTDs were relatively understudied. Mitigation was considered in 174 papers (34%) and adaption strategies in 24 (5%). Amplitude and direction of effects of climate change on malaria and NTDs are likely to vary by disease and location, be non-linear and evolve over time. Available analyses do not allow confident prediction of the overall global impact of climate change on these diseases. For dengue and chikungunya and the group of non-vector-borne NTDs, the literature privileged consideration of current low-burden countries with a high HAQI. No leishmaniasis papers considered outcomes in East Africa. Comprehensive, collaborative and standardised modelling efforts are needed to better understand how climate change will directly and indirectly affect malaria and NTDs.

60 APPLIED LIFE SCIENCES↗

Effect of specific non-pharmaceutical intervention policies on SARS-CoV-2 transmission in the counties of the United States

Non-pharmaceutical interventions (NPIs) remain the only widely available tool for controlling the ongoing SARS-CoV-2 pandemic. We estimated weekly values of the effective basic reproductive number (R eff ) using a mechanistic metapopulation model and associated these with county-level characteristics and NPIs in the United States (US). Interventions that included school and leisure activities closure and nursing home visiting bans were all associated with a median R eff below 1 when combined with either stay at home orders (median R eff 0.97, 95% confidence interval (CI) 0.58–1.39) or face masks (median R eff 0.97, 95% CI 0.58–1.39). While direct causal effects of interventions remain unclear, our results suggest that relaxation of some NPIs will need to be counterbalanced by continuation and/or implementation of others.

60 APPLIED LIFE SCIENCES↗

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗

Impacts of Suppressing Excessive Light Rain on Aerosol Radiative Effects and Health Risks

Global climate models (GCMs) have been used widely to study radiative forcing and health risks of aerosols. A recent study using two GCMs found that light rain plays a dominant role in controlling aerosol loading. However, “too much light rain and too little heavy rain” is a longstanding bias in GCMs. It is unclear how much light rain affects aerosol-cloud-radiation interactions and health risks from air pollution. Here, in this work, we show that, with the correction of the rainfall intensity spectrum in the National Center for Atmospheric Research Community Atmosphere Model version 5.3 by introducing a stochastic deep convection scheme, the reduced frequency of light rain (1–20 mm d -1 ) results in changes of aerosol direct radiative effects (DRE) of up to -0.5 ± 0.03 W/m 2 and aerosol cloud radiative effects (CRE) of up to -0.9 ± 0.03 W/m 2 . The total (CRE + DRE) radiative effects of light rain-mediated aerosol changes exceed the present-day anthropogenic forcing of aerosols relative to preindustrial levels from the Coupled Model Intercomparison Project (CMIP5&6) models. However, the correction of the rainfall intensity spectrum has little effect on anthropogenic aerosol forcing (defined as the radiative perturbation due to changes in aerosol concentrations between the industrial era and preindustrial levels). Due to increased exposure to fine particulates (PM 2.5 ), the estimated global total premature mortality is much higher than previously estimated, by 300,000 ± 60,000 deaths per year, and is more severe in populous regions such as India and China. The findings in this study highlight the need to understand uncertainties in radiative effects and health risks of aerosols due to simulation biases of precipitation in GCMs.

54 ENVIRONMENTAL SCIENCES↗

Direct Observation of Room–Temperature Magnetic Skyrmion Motion Driven by Ultra–Low Current Density in Van Der Waals Ferromagnets

The recent discovery of room-temperature ferromagnetism in 2D van der Waals (vdW) materials, such as Fe 3 GaTe 2 (FGaT), has garnered significant interest in offering a robust platform for 2D spintronic applications. Various fundamental operations essential for the realization of 2D spintronics devices are experimentally confirmed using these materials at room temperature, such as current-induced magnetization switching or tunneling magnetoresistance. Nevertheless, the potential applications of magnetic skyrmions in FGaT systems at room temperature remain unexplored. In this work, the current-induced generation of magnetic skyrmions in FGaT flakes employing high-resolution magnetic transmission soft X-ray microscopy is introduced, supported by a feasible mechanism based on thermal effects. Furthermore, direct observation of the current-induced magnetic skyrmion motion at room temperature in FGaT flakes is presented with ultra-low threshold current density. This work highlights the potential of FGaT as a foundation for room-temperature-operating 2D skyrmion device applications.

2D ferromagnets↗

Observation of the Electromagnetic Field Effect via Charge-Dependent Directed Flow in Heavy-Ion Collisions at the Relativistic Heavy Ion Collider

The deconfined quark-gluon plasma (QGP) created in relativistic heavy-ion collisions enables the exploration of the fundamental properties of matter under extreme conditions. Noncentral collisions can produce strong magnetic fields on the order of 10 18 G , which offers a probe into the electrical conductivity of the QGP. In particular, quarks and antiquarks carry opposite charges and receive contrary electromagnetic forces that alter their momenta. This phenomenon can be manifested in the collective motion of final-state particles, specifically in the rapidity-odd directed flow, denoted as v 1 ( y ) . Here, we present the charge-dependent measurements of d v 1 / d y near midrapidities for π ± , K ± , and p ( p ¯ ) in Au + Au and isobar ( Ru 44 96 + Ru 44 96 and Zr 40 96 + Zr 40 96 ) collisions at s NN = 200 GeV , and in Au + Au collisions at 27 GeV, recorded by the STAR detector at the Relativistic Heavy Ion Collider. The combined dependence of the v 1 signal on collision system, particle species, and collision centrality can be qualitatively and semiquantitatively understood as several effects on constituent quarks. While the results in central events can be explained by the u and d quarks transported from initial-state nuclei, those in peripheral events reveal the impacts of the electromagnetic field on the QGP. Our data put valuable constraints on the electrical conductivity of the QGP in theoretical calculations. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Electrostatic modulation of the lateral carrier density profile in field effect devices with nonlinear dielectrics

The properties of two-dimensional (2D) electronic systems are often effectively controlled using electrostatic gating. The geometry of such field effect devices influences the effectiveness of the gate and the carrier density profile in the 2D device. Here, in this work, we analyze the gate-induced spatial variations in the lateral carrier density in patterned LaAlO 3 /SrTiO 3 devices. We model the electrostatics of the 2D interface using the Thomas-Fermi approximation and compute the gate-induced charge distribution at the interface. We show that the electric field lines generated by the gate are focused at the edges of the device, causing an increased depletion near its edges. This effect is accentuated in LaAlO 3 /SrTiO 3 due to the large, nonlinear dielectric constant of the substrate, and the large distance between the gate electrode and the interface. We experimentally demonstrate one consequence of this effect by directly imaging current distributions in gated heterostructures, finding that insulating regions nucleate at the edges of the device due to the gate. Our results suggest that device geometry and choice of dielectric materials control the charge distribution in 2D systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Improved Dust Representation and Impacts on Dust Transport and Radiative Effect in CAM5

Dust transport and spatial distribution are poorly represented in current global climate models (GCMs) including the Community Atmosphere Model version 5 (CAM5). Particularly, models lack explicit representation of super-coarse dust, which may have important implications for dust radiative forcing and impacts on biogeochemistry. A nine-mode version of the modal aerosol model (MAM9) has been developed to address these issues. In this new aerosol scheme, four dust modes have been designed to treat dust particles of sizes up to 20 μm. The MAM9-simulated results are compared with those from the default four-mode version of MAM (MAM4) and also with the in situ surface measurements of dust concentration and deposition flux, satellite-retrieved dust extinction profile, and in situ vertical measurements of dust concentrations from the NASA Atmosphere Tomography Mission (ATom). Overall, MAM9 improves the dust representation in remote regions while maintaining reasonably good results near the dust source regions. In addition, MAM9 reduces the fine dust burden and increases the coarse dust burden globally. The increased coarse dust burden has slightly increased the dust direct radiative effect by 0.01 W m –2 while it enhanced dust indirect radiative effect by 0.36 W m –2 , globally.

58 GEOSCIENCES↗

Small-scale Assessment of Simplified Ceramic Waste Form Processing

The feasibility of directly processing glass-bonded sodalite ceramic waste form materials by heating a mixture of Zeolite 4A, chloride salt, and sodium borosilicate binder glass was demonstrated by generating laboratory-scale materials. This direct processing method eliminates pre-setting the moisture content of the Zeolite 4A, eliminates the step of occluding salt in the prepared Zeolite 4A prior to processing, and can be conducted using larger particle sizes of crushed Zeolite 4A and crushed borosilicate glass than those called for in the current method. These simplifications are expected to facilitate material transfer and handling in a hot cell or controlled atmosphere environment and be more readily implemented at large scale than the current method. Most materials made to assess these simplifications were directly processed at 925 °C for two hours in an argon atmosphere glovebox, but one material was processed at 925 °C for four hours and one material was processed at 880 °C for two hours. Sodalite was generated and became microencapsulated by the binder glass in all materials. The microstructures were uniform throughout each product, were similar in all products, and were similar to the microstructures of materials made previously using the pressureless consolidation or hot isostatic pressing methods. Various formulations showed the efficiency of sodalite generation was not sensitive to the salt-to-Zeolite 4A ratio or salt-to-glass mass ratio, although a greater relative mass of glass is required to encapsulate sodalite generated from large particles of aggregated Zeolite 4A. The upper limit of salt loadings that can be effectively processed remains to be determined. The effectiveness of direct processing provided new insights into the conversion mechanism. The salt was likely dissolved into the glass that transported NaCl into the Zeolite 4A aggregates and sodalite was generated in situ as NaCl migrated from the outside of the aggregate inward. Other salt cations (e.g., potassium, strontium, cesium, and probably lithium) remain dissolved in the glass encapsulating the zeolite/sodalite domains. When the glass solidifies during cooling, small halite inclusion phases form in glass within sodalite domains and large mixed salt inclusions form in glass surrounding the sodalite due to the low solubility of chloride in the (solid) glass. Other salt cations were oxidized during processing and formed inclusions in the bulk glass (e.g., neodymium). Initial degradation tests show the dissolution behavior of directly processed CWF (SCWF) materials is similar to CWF materials made using different methods.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Imaging Nanoscale Energy Transport and Conversion with Ultrafast Electron Microscopy (Final Technical Report)

Light-matter interactions are ubiquitous in nature and reside at the heart of innumerable technologies. The cascade of processes that occur when a material absorbs a photon of light are exceedingly complex and are interwoven in both space and time, rendering precise determination of the atomic-scale and ultrafast mechanisms immensely challenging. The advent of methods for generating short pulses of light several decades ago led to major advances in understanding the initial moments of light absorption and the resultant effects, though directly interrogating the response of the atoms within the material continued to prove challenging. More recently, methods for generating ultrashort pulses of X-rays and fast electrons have opened the way to probing photoinduced structural dynamics of a wide range of matter in multiple phases. An especially promising laboratory-scale method is ultrafast electron microscopy (UEM), wherein the modalities of conventional transmission electron microscopes (imaging, diffraction, spectroscopy) are extended into the femtosecond temporal regime. Here, the ultrafast imaging and diffraction modalities of UEM were used to study the transient structural aspects of photoexcitation of semiconducting materials (e.g., spatially-resolved electron-phonon coupling, excitation and emission of acoustic phonons, and discrete nanoscale scattering processes). The project had three main objectives: (1) determination of the excitation mechanisms of dense, hypersonic charge-carrier waves and the spatially mediated means by which they couple to the lattice via coherent phonon emission, especially with UEM imaging, wherein effects of nanoscale structural and morphological features on the coupling and relaxation dynamics are expected to dictate nucleation sites and preferred wave vectors, (2) elucidation of photoinduced acoustic-phonon seeding, emergence, propagation, and decay over nanoscale crystal regions and especially with respect to local strain fields and atomic-scale disruptions in lattice order, and (3) interwoven with the first two were efforts aimed at realizing combined angstrom-femtosecond spatiotemporal imaging with UEM. The outcomes and impacts of this project were the generation of new knowledge with respect to fundamental light-matter interactions and, especially, the spatially-mediated excitation and evolution of the structural response of materials following coherent photoexcitation. Importantly, the spatial and temporal resolutions of the UEM imaging modalities used are well-suited for such studies and enable spatially-resolved mechanisms to be determined as a function of atomic order, structural features, and morphology. In addition, ultrafast crystallographic measurements were used to correlate real- and reciprocal-space dynamics in order to determine atomic-scale preferential wave vectors and ultrafast scattering mechanisms, especially as dictated by specimen boundary conditions. The obtained results, as detailed in peer-reviewed publications and presentations, illustrate the importance of ultrafast, angstrom-scale real-space imaging for developing a comprehensive understanding of energy transport and conversion in materials.

47 OTHER INSTRUMENTATION↗

Two pathways to understanding electron transfer in reaction centers from photosynthetic bacteria: A comparison of Rhodobacter sphaeroides and Rhodobacter capsulatus mutants

The rates, yields, mechanisms and directionality of electron transfer (ET) are explored in twelve pairs of Rhodobacter (R.) sphaeroides and R. capsulatus mutant RCs designed to defeat ET from the excited primary donor (P*) to the A-side cofactors and re-direct ET to the normally inactive mirror-image B-side cofactors. In general, the R. sphaeroides variants have larger P + H B - yields (up to similar to ~90%) than their R. capsulatus analogs (up to similar to ~60%), where H B is the B-side bacteriopheophytin. Substitution of Tyr for Phe at L-polypeptide position L181 near B B primarily increases the contribution of fast P* → P + B B - → P + H B - two-step ET, where B-B is the "bridging" B-side bacteriochlorophyll. The second step (similar to ~6-8 ps) is slower than the first (similar to ~3-4 ps), unlike A-side two-step ET (P* → P + B A - → P + H A - ) where the second step (similar to ~1 ps) is faster than the first (similar to ~3-4 ps) in the native RC. Substitutions near H B , at L185 (Leu, Trp or Arg) and at M-polypeptide site M133/131 (Thr, Val or Glu), strongly affect the contribution of slower (20-50 ps) P* → P + H B - one-step superexchange ET. Here, both ET mechanisms are effective in directing electrons "the wrong way" to H B and both compete with internal conversion of P* to the ground state (similar to ~200 ps) and ET to the A-side cofactors. Collectively, the work demonstrates cooperative amino-acid control of rates, yields and mechanisms of ET in bacterial RCs and how A- vs. B-side charge separation can be tuned in both species.

Charge Separation↗

High-temperature anomalous Hall effect driven by frustrated spin fluctuations in the antiferromagnetic delafossite metal PdCrO 2

Metallic delafossite oxides are of exceptional interest due to their ultraclean metallic transport. In the case of PdCrO 2 , this arises in a triangular-lattice antiferromagnet, creating a unique opportunity to study frustrated magnetism in a very clean metal. Here, we combine a chemical vapor transport crystal growth approach with magnetic, thermodynamic, magnetotransport, and neutron scattering measurements to elucidate the striking anomalous Hall effect (AHE) in antiferromagnetic PdCrO 2 . The unconventional AHE (with anomalous Hall conductivity ~10 5 Ω −1 cm −1 ) and a large positive magnetoresistance effect (>1,000%) are shown to exhibit complex temperature dependencies, persisting to almost seven times the Néel temperature (~250 K). These effects are directly compared to elastic neutron scattering, inelastic neutron scattering, and neutron magnetic pair distribution function data, establishing unambiguous links between anomalous magnetotransport properties and directly probed short-range spin fluctuations. The latter occur over a notably broad temperature range due to geometrical magnetic frustration. Connecting to recent experimental and theoretical developments, these findings are discussed in terms of a temperature-dependent interplay between chiral spin order and chiral spin fluctuations, significantly elucidating the high-temperature anomalous magnetotransport in such compounds.

anomalous Hall effect↗

Emerging Strategies for Modifying Lignin Chemistry to Enhance Biological Lignin Valorization

Biological lignin valorization represents a promising approach contributing to sustainable and economic biorefineries. Here, the low level of valuable lignin–derived products remains a major challenge hindering the implementation of microbial lignin conversion. Lignin's properties play a significant role in determining the efficiency of lignin bioconversion. To date, despite significant progress in the development of biomass pretreatment, lignin fractionation, and fermentation over the last few decades, little efforts have gone into identifying the ideal lignin substrates for an efficient microbial metabolism. In this Minireview, emerging and state–of–the–art strategies for biomass pretreatment and lignin fractionation are summarized to elaborate their roles in modifying lignin structure for bioconversion. Fermentation strategies aimed at enhancing lignin depolymerization for microbial utilization are systematically reviewed as well. With an improved understanding of the ideal lignin structure elucidated by comprehensive metabolic pathways and/or big data analysis, modifying lignin chemistry could be more directional and effective. Ultimately, together with the progress of fermentation process optimization, biological lignin valorization will become more competitive in biorefineries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modeling the effect of wind speed and direction shear on utility‐scale wind turbine power production

Abstract Wind speed and direction variations across the rotor affect power production. As utility‐scale turbines extend higher into the atmospheric boundary layer (ABL) with larger rotor diameters and hub heights, they increasingly encounter more complex wind speed and direction variations. We assess three models for power production that account for wind speed and direction shear. Two are based on actuator disc representations, and the third is a blade element representation. We also evaluate the predictions from a standard power curve model that has no knowledge of wind shear. The predictions from each model, driven by wind profile measurements from a profiling LiDAR, are compared to concurrent power measurements from an adjacent utility‐scale wind turbine. In the field measurements of the utility‐scale turbine, discrete combinations of speed and direction shear induce changes in power production of −19% to +34% relative to the turbine power curve for a given hub height wind speed. Positive speed shear generally corresponds to over‐performance and increasing magnitudes of direction shear to greater under‐performance, relative to the power curve. Overall, the blade element model produces both higher correlation and lower error relative to the other models, but its quantitative accuracy depends on induction and controller sub‐models. To further assess the influence of complex, non‐monotonic wind profiles, we also drive the models with best‐fit power law wind speed profiles and linear wind direction profiles. These idealized inputs produce qualitative and quantitative differences in power predictions from each model, demonstrating that time‐varying, non‐monotonic wind shear affects wind power production.

Energy & Fuels↗

Ectomycorrhizal fungal diversity interacts with soil nutrients to predict plant growth despite weak plant-soil feedbacks

Background and aims Plant-soil feedbacks are the result of multiple abiotic and biotic mechanisms. However, few studies have addressed how feedbacks vary based on abiotic context or attempted to identify microbiota responsible for feedbacks. In this work, we investigated whether plant-soil feedbacks of an ectomycorrhizal tree (Quercus macrocarpa) varied based on soil nutrient status and whether fungal community composition and diversity could explain feedback patterns. Furthermore, we inoculated Q. macrocarpa seedlings with field-sampled soils taken from five soil origins – including heterospecific and conspecific trees and an old field – which were profiled using fungal DNA metabarcoding.Results Despite finding that soils associated with different hosts harbored distinct fungal communities and that fungal communities were predictive of plant growth, we did not find any significant plant-soil feedbacks regardless of fertilization status. We did find that the growth promotive effect associated with ectomycorrhizal OTU diversity was weakened with fertilization, suggesting context-dependent relations between plant growth and a guild of fungal mutualists. Our results demonstrate that the host-specific accumulation of functionally important soil microbes is not always sufficient to drive observable plant-soil feedbacks. Our data provide support for a role for ECM fungal diversity in mediating plant growth responses, though it is unclear whether this effect is direct or indirect.

59 BASIC BIOLOGICAL SCIENCES↗