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DOE OSTI2025

Competition response of cloud supersaturation explains diminished Twomey effect for smoky aerosol in the tropical Atlantic

The Twomey effect brightens clouds by increasing aerosol concentrations, which activates more droplets and decreases cloud supersaturation in response to more competition for water vapor. To quantify this competition response, we used marine low cloud observations in clean and smoky conditions at Ascension Island in the tropical South Atlantic during the Layered Aerosol Smoke Interactions with Cloud (LASIC) campaign. These observations show similar increases in droplet number for increased accumulation-mode particles from surface-based and satellite cloud retrievals, demonstrating the importance of below-cloud aerosol measurements for retrieving aerosol–cloud interactions (ACI) in clean and smoky aerosol conditions. Four methods for estimating cloud supersaturation from aerosol–cloud measurements were compared, with cloud scene-based and parcel-based methods showing sufficient variability for a strong dependence on both aerosol accumulation number concentration and cloud-base updraft velocities. Decomposing aerosol-related changes in cloud albedo and optical depth shows the calculated competition response accounts for dampening the activation response by 12 to 35%, explaining the diminished Twomey effect at high aerosol concentrations observed for smoky conditions at LASIC and previously around the world. This result was consistent for independent supersaturation retrievals by cloud scene-based droplet number and cloud condensation nuclei and parcel-based multimode size-resolving Lagrangian methods. Translating aerosol effects to local radiative forcing with clean conditions as a proxy for preindustrial and smoky conditions for present-day showed that the competition response reduces cooling from the Twomey radiative forcing by 12 to 35%, providing an essential process-specific constraint for improving the representation of aerosol competition in climate model simulation of indirect aerosol forcing.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1996

Development of a Rational Modeling Approach for the Design, and Optimization of the Multifiltration Unit

This thesis includes the development and verification of an adsorption model for analysis and optimization of the adsorption processes within the International Space Station multifiltration beds. The fixed bed adsorption model includes multicomponent equilibrium and both external and intraparticle mass transfer resistances. Single solute isotherm parameters were used in the multicomponent equilibrium description to predict the competitive adsorption interactions occurring during the adsorption process. The multicomponent equilibrium description used the Fictive Component Analysis to describe adsorption in unknown background matrices. Multicomponent isotherms were used to validate the multicomponent equilibrium description. Column studies were used to develop and validate external and intraparticle mass transfer parameter correlations for compounds of interest. The fixed bed model was verified using a shower and handwash ersatz water which served as a surrogate to the actual shower and handwash wastewater.

Hand, David W.↗

NASA NTRS1998

Factors Affecting Fiber Design and Selection for Advanced Ceramic Composites

Structural Ceramic Matrix Composites (CMC) have the potential for application in the hot sections of a variety of advanced propulsion and power systems. It is therefore necessary to have a general understanding of the key properties of CMC and Reinforcing Fibers. This need is complicated by the wide variety of application conditions and structural requirements for which CMC's will be used, and the proprietary concerns of the design engineers. CMC's, to be successful, must display properties which are competitive with the currently used high temperature structural materials: (i.e., Iron and Nickel based superalloys, tough monolithic ceramics, and carbon/carbon composites.) Structural CMC offers several areas of competition: (1) performance, (i.e., strength and strength retention, creep resistance, and thermal conductivity), (2) reliability (i.e., environmental durability, and damage tolerance) and (3) processing (i.e., capability for varying sizes and shapes, and cost effective fabrication). The presentation further discusses, and illustrates with fiber and CMC data the key fiber properties and processes which strongly affect each CMC area of competition. The presentation further discusses the current knowledge of the important factors which control the key fiber properties. A design guidelines for the optimum fiber characteristics is developed, and the currently available fibers are compared against those guidelines.

DiCarlo, James A.↗

DOE OSTI2021

Comprehensive process and environmental impact analysis of integrated DBD plasma steam methane reforming

Utilization of electricity generated from renewable sources to obtain hydrogen, H 2 , is of critical importance to decrease the overall carbon footprint. Here in this work, integration of a dielectric discharge barrier (DBD) plasma reactor to convert low calorific value gas, such as landfill gas or coal mine gas into hydrogen, into the existing steam methane reforming (SMR) technology was evaluated using process design considerations. In particular, a DBD-enhanced catalytic SMR reactor was modeled to operate at near atmospheric pressure and 500 °C sequentially with the conventional reformer to obtain ~ 65 kmol/hr H2 for distributed production. This allowed decreasing the size of the conventional reformer albeit at the increased overall electricity consumption. Calculated process economics showed that only at an electricity cost of less than $0.004/kWh does the hybrid DBD plasma process derived H 2 price become competitive with that of the conventional SMR. A Life Cycle Assessment framework was used to compare environmental impacts from the conventional SMR, hybrid DBD SMR and hybrid DBD SMR utilizing only onshore wind-derived electricity. Larger environmental impacts in the plasma reformer were obtained due to the use of electricity for the plasma reforming operation, which was modeled as coming from the typical U.S. grid mix. Utilizing only 100% wind-derived electricity provided certain environmental benefits, except for the ecotoxicity impact where the wind power scenario modeled here only reduced ecotoxicity impacts associated with electricity by 30%.

08 HYDROGEN↗

DOE OSTI2024

Competing Radical and Molecular Channels in the Unimolecular Dissociation of Methylformate

The thermal dissociation of methylformate has been characterized by numerous experimental and theoretical studies that all seem to agree that the lowest energetically accessible process is a 3-center H-atom transfer that leads to the molecular products CH3OH 3 OH + CO. However, these literature studies seem to be at odds with regards to the role of other competing molecular eliminations and bond-fission processes and therefore a complete and resolved mechanistic picture of methylformate thermal dissociation still eludes us. In this work, we have performed high-level electronic structure theory calculations to characterize the energetics of other overlooked molecular and radical processes that can originate on the complex CH3OCHO 3 OCHO potential energy surface (PES). The present calculations do indeed confirm that the lowest energy process accessible on this PES is molecular elimination to form CH3OH 3 OH + CO. However, unlike prior theoretical studies, the present calculations reveal that the second lowest energy process is a 5-center concerted elimination process that leads to the direct formation of H2 2 + CH2O 2 O + CO. We also note that HCO2 2 from the lowest-lying bond fission has two energetically comparable electronic states (of 2 B 2 and 2 A 1 symmetry). Furthermore, the barrier for H-atom migration of CH3OCHO 3 OCHO to form the carbene (CH3OCOH) 3 OCOH) is similar to that for the direct 4-center elimination process leading to CH2O 2 O + CH2O 2 O characterized in prior literature studies. Radical and molecular pathways to CH3 3 + HOCO and CH4 4 + CO2 2 can also be facilitated from this carbene. Master equation calculations were performed to characterize the competition between the various molecular and radical processes on this more elaborate CH3OCHO 3 OCHO PES. The results of the present theoretical analyses were used to resolve outstanding questions on the role of secondary radical- initiated reactions in characterizing prior literature experimental studies.

Chemical Kinetics↗

DOE OSTI2022

Structure-Based Prototyping of Allosteric Inhibitors of Human Uridine/Cytidine Kinase 2 (UCK2)

Pyrimidine nucleotide biosynthesis in humans is a promising chemotherapeutic target for infectious diseases caused by RNA viruses. Because mammalian cells derive pyrimidine ribonucleotides through a combination of de novo biosynthesis and salvage, combined inhibition of dihydroorotate dehydrogenase (DHODH; the first committed step in de novo pyrimidine nucleotide biosynthesis) and uridine/cytidine kinase 2 (UCK2; the first step in salvage of exogenous nucleosides) strongly attenuates viral replication in infected cells. However, while several pharmacologically promising inhibitors of human DHODH are known, to date there are no reports of medicinally viable leads against UCK2. Here we use structure-based drug prototyping to identify two classes of promising leads that non-competitively inhibit UCK2 activity. In the process we have identified a hitherto unknown allosteric site at the inter-subunit interface of this homotetrameric enzyme. By reducing the kcat of human UCK2 without altering its KM, these new inhibitors have the potential to enable systematic dialing of the fractional inhibition of pyrimidine salvage to achieve the desired antiviral effect with minimal host toxicity.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Calcium Cosalt Addition to Alter the Cation Solvation Structure and Enhance the Ca Metal Anode Performance

Accessing the energy density and sustainability of calcium metal batteries requires mastering reversible calcium electrodeposition through electrolyte design. Several electrolytes support reversible, ambient temperature deposition but at utilization and rate too low for practical applications. These challenges stem from solvation structures characterized by either high barriers for cation desolvation or thermodynamic instability, leading to parasitic decomposition of the salt and solvent. The optimal solvation structure for the effective delivery of calcium to the electrode interface is not known. In this work, we show that adding a relatively small amount of a weakly associating calcium salt (calcium carba-closo-dodecaborate) to an otherwise strongly associated solution (calcium borohydride in tetrahydrofuran) produces a surprising population of fully solvent-coordinated Ca2+ cations in the form of solvent-separated ion pairs (SSIPs). We further demonstrate that the formation of these SSIPs beneficially impacts the kinetics and thermodynamics of calcium electrodeposition, revealing the unexpected finding that direct coordination of Ca2+ by the BH4– anion limits the electrodeposition process. These findings reveal how the competition between solvent and anion coordination to Ca2+ affects calcium deposition kinetics and cycling stability, setting the stage for a new calcium electrolyte design based on mixed anion electrolytes.

Landers, Alan T.↗

DOE OSTI2021

The challenges of electrolytic valorization of carbon dioxide

Electroreduction of carbon dioxide is an enabling technology that can produce valuable chemicals, such as C 1 (for example, formic acid and carbon monoxide) and C 2 chemicals (for example, ethylene and ethanol), with a minimal or even negative carbon footprint. Now, a techno-economic analysis shows that only the C 1 products can achieve competitive prices, while substantial improvements in process economics are needed for C 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Catalyst synthesis under CO 2 electroreduction favours faceting and promotes renewable fuels electrosynthesis

The electrosynthesis of C 2+ hydrocarbons from CO 2 has garnered recent attention in light of the relatively high market price per unit energy input. Today’s low selectivities and stabilities towards C 2+ products at high current densities curtail system energy efficiency, which limits their prospects for economic competitiveness. Here we present a materials processing strategy based on in situ electrodeposition of copper under CO 2 reduction conditions that preferentially expose and maintain Cu(100) facets, which favour the formation of C 2+ products. We observe capping of facets during catalyst synthesis and achieve control over faceting to obtain a 70% increase in the ratio of Cu(100) facets to total facet area. We report a 90% Faradaic efficiency for C 2+ products at a partial current density of 520 mA cm –2 and a full-cell C 2+ power conversion efficiency of 37%. We achieve nearly constant C2H4 selectivity over 65 h operation at 350 mA cm –2 in a membrane electrode assembly electrolyser.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Coupled nuclear–electronic decay dynamics of O2 inner valence excited states revealed by attosecond XUV wave-mixing spectroscopy

Multiple Rydberg series converging to the $O_2^+$ c $^{4}Σ^{-}_{u}$ state, accessed by 20-25 eV extreme ultraviolet (XUV) light, serve as important model systems for the competition between nuclear dissociation and electronic autoionization. The dynamics of the lowest member of these series, the $3sσ_g $ state around 21 eV, has been challenging to study owing to its ultra-short lifetime (<10 fs). Here, we apply transient wave-mixing spectroscopy with an attosecond XUV pulse to investigate the decay dynamics of this electronic state. Lifetimes of 5.8 ± 0.5 fs and 4.5 ± 0.7 fs at 95% confidence intervals are obtained for v = 0 and v = 1 vibrational levels of the 3s Rydberg state, respectively. A theoretical treatment of predissociation and electronic autoionization finds that these lifetimes are dominated by electronic autoionization. The strong dependence of the electronic autoionization rate on the internuclear distance because of two ionic decay channels that cross the 3s Rydberg state results in the different lifetimes of the two vibrational levels. The calculated lifetimes are highly sensitive to the location of the 3s potential with respect to the decay channels; by slight adjustment of the location, values of 6.2 and 5.0 fs are obtained computationally for the v = 0 and v = 1 levels, respectively, in good agreement with experiment. Overall, an intriguing picture of the coupled nuclear-electronic dynamics is revealed by attosecond XUV wave-mixing spectroscopy, indicating that the decay dynamics are not a simple competition between isolated autoionization and predissociation processes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Estimated timescales for wet deposition of organic compounds as a function of Henry's law constants

Atmospheric organic compounds may deposit to Earth's surfaces via dry deposition, driven by concentration gradients, and wet deposition, driven by the scavenging of compounds by precipitation. Their removal by deposition has downstream impacts on concentrations of secondary organic aerosol by removing potential aerosol precursors that would otherwise oxidize to form particulate matter. The impact of deposition processes can consequently be considered as competition between rates of oxidation and deposition, but timescales for deposition are not well constrained. While timescales for dry deposition have been estimated and experimentally validated in the past, understanding of wet deposition of organics is still very limited. In this work, we estimate the wet deposition timescale for gas-phase organic compounds in the atmosphere as a function of Henry's law constants, H, using real-world precipitation frequency and size distributions at five globally-distributed sites. The wet deposition timescale decreases significantly with the increase of H until reaching a stable minimum for compounds with H > 10 5 M per atm. We estimate that the median wet deposition timescale for highly soluble gases is approximately 5 hours during a continuous rain event for all sites. However, median estimated timescales ranged from 80 to 200 hours, depending on location. Timescales are found to depend primarily on the frequency and duration of precipitation events rather than their intensity or size characteristics. Based on these data, we demonstrate that timescales for wet deposition of gases can be estimated at any given location using only basic precipitation information, without detailed or high-precision measurements.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Three-dimensional particle-in-cell simulations of laser-driven multiradiation sources based on double-layer targets

Double-layer targets (DLTs), made of a low-density foam on top of a solid substrate, can efficiently convert the energy of a high-intensity laser to provide sources of photons and protons. We investigate a 30-fs pulse with a peak intensity of I ~ 8.7×10 20 W/cm 2 and a peak power of ~120 TW interacting with a DLT using three-dimensional (3D) particle-in-cell simulations. We focus on providing quantitative results in full 3D geometry on the foam thickness dependence; on the competition between two photon-generating processes in DLTs, i.e., nonlinear inverse Compton scattering (NICS) and bremsstrahlung (BS); and on the acceleration of protons via enhanced target-normal sheath acceleration. Here, we discuss conversion efficiency, average energy, and angular distributions of such multiradiation sources. We find that NICS can prevail over BS if the DLT's substrate is thin enough (~µ⁢m) and that the optimal foam thickness that maximizes the conversion efficiency in NICS and BS photons and the proton cutoff energy, among those considered, is the same (15µ⁢m). These results show that DLTs constitute an excellent tool for developing relatively compact and optimized laser-driven multicomponent radiation sources.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Batteries Annual Progress Report (FY2019)

The Vehicle Technologies Office (VTO) of the Department of Energy (DOE) conducts research and development (R&D) on advanced transportation technologies that would reduce the nation’s use of imported oil and would also lead to reductions in harmful emissions. Technologies supported by VTO include electric drive components such as advanced energy storage devices (primarily batteries), power electronics and electric drive motors, advanced structural materials, energy efficient mobility systems, advanced combustion engines, and fuels. VTO is focused on funding early-stage high-reward/high-risk research to improve critical components needed for more fuel efficient (and cleaner-operating) vehicles. One of the major VTO objectives is to enable U.S. innovators to rapidly develop the next generation of technologies that achieve the cost, range, and charging infrastructure necessary for the widespread adoption of plug-in electric vehicles (PEVs). An important prerequisite for the electrification of the nation’s light duty transportation sector is development of more cost-effective, longer lasting, and more abuse-tolerant PEV batteries. One of the ultimate goals of this research, consistent with the current vehicle electrification trend, is an EV which can provide the full driving performance, convenience, and price of an internal combustion engine (ICE) vehicle. To achieve this, VTO has established the following overarching goal (Source: FY2021 Congressional Budget Justification1): …identify new battery chemistry and cell technologies with the potential to reduce the cost of electric vehicle battery packs by more than half, to less than $100/kWh (ultimate goal is $60/kWh battery cell cost), increase range to 300 miles, and decrease charge time to 15 minutes or less by 2028. VTO works with key U.S. automakers through the United States Council for Automotive Research (USCAR) – an umbrella organization for collaborative research consisting of Fiat Chrysler Automobiles (FCA), the Ford Motor Company, and General Motors. Collaboration with automakers through the partnership known as U.S. Driving Research and Innovation for Vehicle Efficiency and Energy Sustainability (U.S. DRIVE) attempts to enhance the relevance and the success potential of its research portfolio. VTO competitively selects projects for funding through funding opportunity announcements (FOAs). Directly-funded work at the national laboratories are awarded competitively through a lab-call process. During the past year, VTO continued R&D in support of PEVs. Stakeholders for VTO R&D include universities, national laboratories, other government agencies and industry (including automakers, battery manufacturers, material suppliers, component developers, private research firms, and small businesses). This document summarizes the progress of VTO battery R&D projects supported during the fiscal year 2019 (FY 2019).

25 ENERGY STORAGE↗

DOE OSTI2024

Cas9 deletion of lutein biosynthesis in the marine alga Picochlorum celeri reduces photosynthetic pigments while sustaining high biomass productivity

Domestication of algae for food and renewable biofuels remains limited by the low photosynthetic efficiencies of processes that have evolved to be competitive for optimal light capture, incentivizing the development of large antennas in light-limiting conditions, thus decreasing efficient light utilization in cultivated ponds or photobioreactors. Reducing the pigment content to improve biomass productivity has been a strategy discussed for several decades and the ability to reduce pigment significantly is now fully at hand thanks to the widespread use of genome editing tools. Picochlorum celeri is one of the fastest growing marine algae identified and holds particular promise for outdoor cultivation, especially in saline water and warm climates. We show that while chlorophyll b is essential to sustain high biomass productivities under dense cultivation, removing Picochlorum celeri’s main carotenoid, lutein, leads to a decreased total chlorophyll content, higher a/ b ratio, reduced functional LHCII cross section and higher maximum quantum efficiencies at lower light intensities, resulting in an incremental increase in biomass productivity and increased PAR-to-biomass conversion efficiency. These findings further strengthen the existing strategies to improve photosynthetic efficiency and biomass production in algae.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1978

The natural and perturbed troposphere

A quantitative assessment of the chemical and climatic effects of industrial emissions into the atmosphere requires an understanding of the complex interactions of species within the atmosphere and of the atmosphere with other physical systems such as the oceans, lithosphere, and biosphere. The concentration of a particular species is determined by competition between various production and loss processes. The abundances of tropospheric gases are examined. The reactions of the members of the oxygen group are considered along with the models which have been developed to describe the involved relationships. Attention is also given to the natural carbon cycle, perturbations to the carbon cycle, the natural nitrogen cycle, perturbations to the nitrogen cycle, the hydrogen group, the sulfur group, and the halogen group.

Stewart, R. W.↗

NASA NTRS1986

One-photon pair annihilation in magnetized relativistic plasmas

In supersonic magnetic fields, electron-positron pairs may annihilate into single photons producing spectral features above 1 MeV. The paper calculates the exact one-photon annihilation rate in the general case where pairs may annihilate from excited Landau states, extending the previous studies which were restricted to pairs in the ground state. Asymptotic expressions for annihilation spectra and rates in the limit of large pair quantum numbers are also derived. It is found that the rate of annihilation from excited states can exceed the rate from the ground state by orders of magnitude in fields less than about 2 x 10 to the 12th G. This allows one-photon annihilation to be competitive with the two-photon process at typical neutron star field strengths. Annihilation spectra from a Maxwellian pair plasma at transrelativistic temperatures show fine structure near threshold on a scale (h/2pi)omega sub B as the result of contributions from individual pair states, which blend into a smooth continuum at higher energies.

Harding, A. K.↗

NASA NTRS1989

The impact history of the solar system - Implications for the origins of atmospheres

The present consideration of the roles played by impacts in the origin and evolution of planetary and satellite atmospheres notes that while small impacts of volatile-rich planetesimals can contribute to a body's volatile inventory, large impacts blow away existing primordial atmospheres and generate main-body outgassing; these processes would have been in greatest competition during the end-stage of accretion. The uncertainties in solar system cratering-record interpretation and event-chronology yield only order-of-magnitude estimates. Temporal fluctuations in the impact rate may be very large, notably in the case of cometary sources, where a factor-of-2 variation is common, and a factor-of-100 variation is entirely possible.

Weissman, P. R.↗

NASA NTRS1991

Continuous fiber-reinforced titanium aluminide composites

An account is given of the fabrication techniques, microstructural characteristics, and mechanical behavior of a lightweight, high service temperature SiC-reinforced alpha-2 Ti-14Al-21Nb intermetallic-matrix composite. Fabrication techniques under investigation to improve the low-temperature ductility and environmental resistance of this material system, while reducing manufacturing costs to competitive levels, encompass powder-cloth processing, foil-fiber-foil processing, and thermal-spray processing. Attention is given to composite microstructure problems associated with fiber distribution and fiber-matrix interfaces, as well as with mismatches of thermal-expansion coefficient; major improvements are noted to be required in tensile properties, thermal cycling effects, mechanical damage, creep, and environmental effects.

Mackay, R. A.↗