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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Mechanistic insights into nitrogen activation on atomic Ru clusters in self-pillared pentasil using operando atomistic models and experimental kinetics

Alternative catalysts to the industrial Haber Bosch process have been of significant interest in the field of heterogeneous catalysis, yet realizing ammonia synthesis under mild conditions (e.g., 300 °C and 10 bar) is challenging due to the low per-pass conversion. One strategy is to promote the associative ammonia synthesis mechanism which eschews direct N-N bond cleavage. Here, in this work, we use self-pillared pentasil, a self-pillared hierarchical zeolite built by thin MFI zeolite nanosheets, as a support for subnanometric Ru clusters to synthesize ammonia. We show that Ru remains well-dispersed during reaction and further demonstrate that ammonia synthesis rates are higher than Cs-Ru/MgO. Reaction kinetics show a positive order in H 2 providing evidence for the associative mechanism, which then becomes negative in H 2 if Ru is allowed to aggregate into nanoparticles. Operando Density Functional Theory models for Ru speciation in SPP, free energy diagrams, and microkinetic modeling were then applied to develop a reaction mechanism that involves sequential hydrogenation of N 2 from metallic Ru clusters. For this hydrogenation to occur, there are site requirements for N 2 to adopt a bridge-bound configuration that facilitates sequential hydrogenation on single sites and metal clusters. These site requirements in turn inform the design of improved zeolite-supported ammonia synthesis catalysts.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ponderomotive recoil for electromagnetic waves

When waves damp or amplify on resonant particles in a plasma, nonresonant particles experience a recoil force that conserves the total momentum between particles and electromagnetic fields. This force is important to understand, as it can completely negate current drive and rotation drive mechanisms that are predicted on the basis of only resonant particles. Here, the existing electrostatic theory of this recoil force is extended to electromagnetic waves. While the result bears close similarity to historical fluid theories of laser–plasma interactions, it now incorporates both resonant and nonresonant particles, allowing momentum conservation to be self-consistently proven. Furthermore, the result is shown to be generally valid for kinetic plasmas, which is verified through single-particle hot-plasma simulations. Here, the new form of the force provides physical insight into the nature of the generalized Minkowski (plasmon) momentum of geometrical optics, which is shown to correspond to the momentum gained by the field and nonresonant particles as the wave is self-consistently ramped up from vanishing amplitude.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Toward a Better Understanding of Ni Coarsening in Solid Oxide Cells: NiH on Ni (111) Examined Using a Combined Theoretical Approach

The coarsening of the Ni particles in the hydrogen electrode of solid oxide cells (SOCs) is an important degradation mechanism. Here, in this paper, density-functional theory and kinetic Monte Carlo methods are used to explore our recent hypothesis that the surface diffusion of NiH may cause faster Ni coarsening in electrolysis cell mode under an overpotential. Using both methods, the diffusion constant or diffusivity of NiH on Ni (111) is determined as the product of the surface coverage and single-molecule diffusivity for the first time considering all possible diffusion paths. It is then determined versus overpotential at the triple-phase boundary of the hydrogen electrode assuming a typical operating temperature of the SOC. Under a significant overpotential, the diffusivity of NiH is found to be sufficiently large to support the above hypothesis that NiH may promote Ni coarsening. However, based on the adsorption configurations identified, the dissociation and reformation of NiH on Ni (111) could occur. Thus, more work is needed to develop a model of Ni coarsening considering both molecular and dissociated forms of NiH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Theories of Relativistic Dissipative Fluid Dynamics

Relativistic dissipative fluid dynamics finds widespread applications in high-energy nuclear physics and astrophysics. However, formulating a causal and stable theory of relativistic dissipative fluid dynamics is far from trivial; efforts to accomplish this reach back more than 50 years. In this review, we give an overview of the field and attempt a comparative assessment of (at least most of) the theories for relativistic dissipative fluid dynamics proposed until today and used in applications.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS2005

Gas Dynamics and Kinetics in the Cometary Coma: Theory and Observations

Our ability to describe the physical state of the expanding coma affects fundamental areas of cometary study both directly and indirectly. In order to convert measured abundances of gas species in the coma to gas production rates, models for the distribution and kinematics of gas species in the coma are required. Conversely, many different types of observations, together with laboratory data and theory, are still required to determine coma model attributes and parameters. Accurate relative and absolute gas production rates and their variations with time and from comet to comet are crucial to our basic understanding of the composition and structure of cometary nuclei and their place in the solar system. We review the gas dynamics and kinetics of cometary comae from both theoretical and observational perspectives, which are important for understanding the wide variety of physical conditions that are encountered.

Combi, Michael R.↗
DOE OSTI2022

Momentum conservation in current drive and alpha-channeling-mediated rotation drive

Alpha channeling uses waves to extract hot ash from a fusion plasma, transferring energy from the ash to the wave. It has been proposed that this process could create a radial electric field, efficiently driving E × B rotation. However, existing theories ignore the nonresonant particles, which play a critical role in enforcing momentum conservation in quasilinear theory. Because cross field charge transport and momentum conservation are fundamentally linked, this non-consistency throws the rotation drive into question. This paper has two main goals. First, we provide a pedantic and cohesive introduction to the recently developed simple, general, self-consistent quasilinear theory for electrostatic waves that explains the torques which allow for current drive parallel to the magnetic field, and charge extraction across it; a theory that has largely resolved the question of rotation drive by alpha channeling. We show how the theory reveals a fundamental difference between the reaction of nonresonant particles to plane waves that grow in time vs steady-state waves that have a nonuniform spatial structure, allowing rotation drive in the latter case while precluding it in the former, and we review the local and global conservation laws that lead to this result. Second, we provide two new results in support of the theory. First, we provide a novel two-particle Hamiltonian model that rigorously establishes the relationship between charge transport and momentum conservation. Second, we compare the new quasilinear theory to the oscillation-center theories of ponderomotive forces, showing how the latter often obscure the time-dependent nonresonant recoil, but ultimately lead to similar results.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Inclusive curvaturelike framework for describing dissipation: Metriplectic 4-bracket dynamics

An inclusive framework for joined Hamiltonian and dissipative dynamical systems that are thermodynamically consistent, i.e., preserve energy and produce entropy, is given. The dissipative dynamics of the framework is based on the metriplectic 4-bracket , a quantity like the Poisson bracket defined on phase space functions, but unlike the Poisson bracket has four slots with symmetries and properties motivated by Riemannian curvature. Metriplectic 4-bracket dynamics is generated using two generators, the Hamiltonian and the entropy, with the entropy being a Casimir of the Hamiltonian part of the system. The formalism includes known previous binary bracket theories for dissipation or relaxation as special cases. Rich geometrical significance of the formalism and methods for constructing metriplectic 4-brackets are explored. Many examples of both finite and infinite dimensions are given.

Physics↗
DOE OSTI2021

Global Theory of Microtearing Modes in the Tokamak Pedestal

The pedestal of H-mode tokamaks displays strong magnetic fluctuations correlated with the evolution of the electron temperature. The microtearing mode (MTM), a temperature-gradient-driven instability that alters magnetic topology, is compatible with these observations. Here we extend the conventional theory of the MTM to include the global variation of the temperature and density profiles. The offset between the rational surface and the location of the pressure gradient maximum (μ) emerges as a crucial parameter for MTM stability. In conclusion, the extended theory matches observations on the Joint European Torus tokamak.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Fundamental Studies of Oxidation Reactions on Model Catalysts. Final report

This report covers the reporting period from 08/15/2003 to 08/31/2019. The research activities were focused on the oxidation of methane, nitric oxide, and propylene in addition to contributions on the kinetics, synthesis, theory and characterization of various catalytic systems. As described in the report, we were able to formulate hypotheses, construct specialized equipment and carry out experimental and theoretical work to test the hypotheses. Major advances were accomplished in the fundamental understanding of these systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Mean force emission theory for classical bremsstrahlung in strongly coupled plasmas

This work presents mean force emission theory, which extends the classical theory of bremsstrahlung emission to strongly coupled plasmas. In the high-frequency limit, the theory reduces to solving for the electron trajectory during a binary collision, but where the electron–ion interactions occur through the potential of mean force. In the low-frequency limit, it uses an autocorrelation formalism that captures effects of multiple collisions and strongly correlated motion. The predictions are benchmarked by comparison with first-principles classical molecular dynamics simulations of a fully ionized hydrogen plasma in which all interactions are repulsive. The comparison shows good agreement up to Coulomb coupling strengths of Γ∼30. The theory improves upon traditional models by including strong coupling effects and systematically including the effect of multiple collisions. Furthermore, mean force emission theory provides evidence that the Drude correction factor commonly used in quantum calculations of optical quantities may not be adequate at strong coupling.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Effective dissipation rate in a Liouvillian-graph picture of high-temperature quantum hydrodynamics

At high temperature, generic strongly interacting spin systems are expected to display hydrodynamics: local transport of conserved quantities, governed by classical partial differential equations like the diffusion equation. I argue that the emergence of this dissipative long-wavelength dynamics from the system's unitary microscopic dynamics is controlled by the structure of the Liouvillian graph of the system's Hamiltonian, that is, the graph induced on Pauli strings by commutation with that Hamiltonian. The Liouvillian graph decomposes naturally into subgraphs of Pauli strings of constant diameter, and the coherent dynamics of these subgraphs determines the rate at which operator weight spreads to long operators. In conclusion, this argument provides a quantitative theory of the emergence of a dissipative effective dynamics from unitary microscopic dynamics; it also leads to an effective model with Hilbert space dimension linear in system size and exponential in the UV cutoff for diffusion.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Degrees of Rate Control in Interconnected Reaction Networks

Overall reactions in interconnected networks exhibit net, forward, and reverse rates that are governed by both constitutive elementary steps in the pathway of interest and branching elementary steps that lead to alternative products. Accordingly, steps in branching pathways exhibit negative net, forward, and reverse degrees of rate control, as they reduce reaction flux to the desired product. We here contextualize the forward and reverse degrees of rate control in terms of kinetic resistances (inverse of rates) and leverage the additive nature of kinetic resistance to decouple kinetic driving forces contributed by constitutive elementary steps and branching points (nodal species) in interconnected networks. Regardless of the network connectivity, forward and reverse degrees of rate control are shown to converge at equilibrium. Away from equilibrium, we identify two critical features of interconnected networks: stoichiometric regularity─condition where all stoichiometric numbers are unity─and pathway symmetry around nodal species─condition where branching pathways share the same rate constants, stoichiometry, and species concentrations/activities─that result in (i) equal forward, reverse, and consequently net degrees of rate control and (ii) forward and reverse degrees of rate control that exhibit constant offsets, respectively, across all extents of reaction. Furthermore, our discourse further provides a mathematical description for the influence of stoichiometric irregularity and pathway asymmetry on forward and reverse degrees of rate control. Altogether, the presented work details the effects of network (inter)connectivity and stoichiometry on reaction kinetics and, in doing so, establishes general protocols for capturing these effects as additive terms in the formulation of forward and reverse degrees of rate control.

10 SYNTHETIC FUELS↗
DOE OSTI2024

Fine-tuning catalytic selectivity by modulating catalyst-environment interactions: CO 2 hydrogenation over Pd-based catalysts

Capturing catalytic behaviors under operational conditions is pivotal to gaining a mechanistic understanding and promoting the design of robust catalysts. The challenge lies in the difficulty of monitoring real-time surface dynamics driven by catalyst-environment interactions. Here, in this work, we introduce a framework based on density functional calculations and kinetic modeling. This framework significantly improves the accuracy of theoretical models’ descriptions of experimental observations by quantifying environmental impacts on surface phases and active sites. CO 2 hydrogenation over Pd-based catalysts is taken as a showcase. The observed selectivity variations of Pd and Pd-M bimetallic catalysts strongly correlate with hydrogen coverage maintained under typical CO 2 hydrogenation conditions. By reducing the amount of surface hydrogen, the selectivity tuned effectively from formic acid toward CO and methanol. This study not only deepens the comprehension of dynamics of active sites under active chemical conditions but also introduces an alternative opportunity for catalytic tuning by modulating catalyst-environment interactions.

03 NATURAL GAS↗
DOE OSTI2025

Examining Ni Coarsening in Solid Oxide Electrolysis Cells by Characterizing NiH on Ni (111) Using a Combined Theoretical Approach

Ni coarsening in the fuel electrode of solid oxide cells (SOCs) is an important degradation mechanism. In this talk, density-functional theory and kinetic Monte Carlo methods are used to explore the hypothesis that the surface diffusion of NiH on Ni may promote Ni coarsening in the SOC operated in electrolysis cell mode. Using both methods and defining the diffusivity as the product of the surface coverage and single-molecule diffusivity, the diffusivity of NiH on Ni (111) is found to be sufficiently large under a significant overpotential to support the above hypothesis. Also, the time between the formation and dissociation of NiH on Ni (111) is predicted to be short at low coverages of H on Ni (111). Thus, significant progress is made toward developing a model of Ni coarsening considering both molecular and dissociated forms of NiH on Ni (111).

density functional theory (DFT)↗
DOE OSTI2023

Theory of the ion–electron temperature relaxation rate in strongly magnetized plasmas

Recent works have shown that strongly magnetized plasmas characterized by having a gyrofrequency greater than the plasma frequency exhibit novel transport properties. One example is that the friction force on a test charge shifts, obtaining components perpendicular to its velocity in addition to the typical stopping power component antiparallel to its velocity. Here, we apply a recent generalization of the Boltzmann equation for strongly magnetized plasmas to calculate the ion–electron temperature relaxation rate. Strong magnetization is generally found to increase the temperature relaxation rate perpendicular to the magnetic field and to cause the temperatures parallel and perpendicular to the magnetic field to not relax at equal rates. This, in turn, causes a temperature anisotropy to develop during the equilibration. Strong magnetization also breaks the symmetry of independence of the sign of the charges of the interacting particles on the collision rate, commonly known as the “Barkas effect.” Furthermore, it is found that the combination of oppositely charged interaction and strong magnetization causes the ion–electron parallel temperature relaxation rate to be significantly suppressed, scaling inversely proportional to the magnetic field strength.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Electron Weibel instability induced magnetic fields in optical-field ionized plasmas

Generation and amplification of magnetic fields in plasmas is a long-standing topic that is of great interest to both plasma and space physics. The electron Weibel instability is a well-known mechanism responsible for self-generating magnetic fields in plasmas with temperature anisotropy and has been extensively investigated in both theory and simulations, yet experimental verification of this instability has been challenging. Recently, we demonstrated a new experimental platform that enables controlled initialization of highly nonthermal and/or anisotropic plasma electron velocity distributions via optical-field ionization. Using an external electron probe bunch from a linear accelerator, the onset, saturation, and decay of the self-generated magnetic fields due to electron Weibel instability were measured for the first time to our knowledge. In this paper, we will first present experimental results on time-resolved measurements of the Weibel magnetic fields in non-relativistic plasmas produced by Ti:Sapphire laser pulses (0.8 μm) and then discuss the feasibility of extending the study to a quasi-relativistic regime by using intense CO 2 (e.g., 9.2 μm) lasers to produce much hotter plasmas.

36 MATERIALS SCIENCE↗