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At least 631 records · Page 35
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Colloidal Stability of PFSA-Ionomer Dispersions. Part I. Single-Ion Electrostatic Interaction Potential Energies

Charged colloidal particles neutralized by a single counterion are increasingly important for many emerging technologies. Attention here is paid specifically to hydrogen fuel cells and water electrolyzers whose catalyst layers are manufactured from a perfluorinated sulfonic acid polymer (PFSA) suspended in aqueous/alcohol solutions. Partially dissolved PFSA aggregates, known collectively as ionomers, are stabilized by the electrostatic repulsion of overlapping diffuse double layers consisting of only protons dissociated from the suspended polymer. We denote such double layers containing no added electrolyte as "single ion". Size-distribution predictions build upon interparticle interaction potential energies from the Derjaguin-Landau-Verwey-Overbeek (DLVO) formalism. However, when only a single counterion is present in solution, classical DLVO electrostatic potential energies no longer apply. Accordingly, here a new formulation is proposed to describe how single-counterion diffuse double layers interact in colloidal suspensions. Part II (Srivastav, H.; Weber, A. Z.; Radke, C. J. Langmuir 2024 DOI: 10.1021/acs.langmuir.3c03904) of this contribution uses the new single-ion interaction energies to predict aggregated size distributions and the resulting solution pH of PFSA in mixtures of n-propanol and water. A single-counterion diffuse layer cannot reach an electrically neutral concentration far from a charged particle. Consequently, nowhere in the dispersion is the solvent neutral, and the diffuse layer emanating from one particle always experiences the presence of other particles (or walls). Thus, in addition to an intervening interparticle repulsive force, a backside osmotic force is always present. With this new construction, we establish that single-ion repulsive pair interaction energies are much larger than those of classical DLVO electrostatic potentials. The proposed single-ion electrostatic pair potential governs dramatic new dispersion behavior, including dispersions that are stable at a low volume fraction but unstable at a high volume fraction and finite volume-fraction dispersions that are unstable with fine particles but stable with coarse particles. Finally, the proposed single-counterion electrostatic pair potential provides a general expression for predicting colloidal behavior for any charged particle dispersion in ionizing solvents with no added electrolyte.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1984

Electrostatic hydrogen-cyclotron wave emission below the hydrogen-cyclotron frequency in the auroral acceleration region

A mechanism is suggested for the excitation of electrostatic ion-cyclotron waves at frequencies below the ion-cyclotron frequency in the midst of the auroral acceleration region, which is assumed to consist of downward moving double layers. The mechanism involves upward flowing ions interacting with a downward flowing background plasma. The upward flowing ions are the ion beams accelerated by the double layer. The downward motion of the background plasma corresponds to a plasma expansion into the density cavity that develops in connection with double layer formation in the acceleration region. The ion-cyclotron waves excited by the counterstreaming flows are doppler shifted to frequencies below the harmonics of the ion cyclotron frequency. It is suggested that such wave emissions could account for some very narrow-banded waves at frequencies below the hydrogen cyclotron frequency that were observed by the S3-3 satellite.

Singh, N.↗
DOE OSTI2016

Impedance of an intense plasma-cathode electron source for tokamak startup

In this study, an impedance model is formulated and tested for the ~1kV, ~1kA/cm 2 , arc-plasma cathode electron source used for local helicity injection tokamak startup. A double layer sheath is established between the high-density arc plasma (n arc ≈ 10 21 m -3 ) within the electron source, and the less dense external tokamak edge plasma (n edge ≈ 10 18 m -3 ) into which current is injected at the applied injector voltage, V inj . Experiments on the Pegasus spherical tokamak show the injected current, I inj , increases with V inj according to the standard double layer scaling I inj ~ V inj 3/2 at low current and transitions to I inj ~ V inj 1/2 at high currents. In this high current regime, sheath expansion and/or space charge neutralization impose limits on the beam density n b ~ I inj /V inj 1/2 . For low tokamak edge density n edge and high I inj , the inferred beam density n b is consistent with the requirement n b ≤ n edge imposed by space-charge neutralization of the beam in the tokamak edge plasma. At sufficient edge density, n b ~ n arc is observed, consistent with a limit to n b imposed by expansion of the double layer sheath. These results suggest that n arc is a viable control actuator for the source impedance.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Distance-dependent dielectric constant at the calcite/electrolyte interface: Implication for surface complexation modeling

Hypothesis: The electrical double layer formed at the mineral/electrolyte interface is often modeled using mean-field approaches based on a continuum description of the solvent whose dielectric constant is assumed to decrease monotonically with decreasing distance to the surface. In contrast, molecular simulations show that the solvent polarizability oscillates near the surface similar to the water density profile - as shown previously, for example, by Bonthuis et al. (D.J. Bonthuis, S. Gekle, R.R. Netz, Dielectric Profile of Interfacial Water and its Effect on Double-Layer Capacitance, Phys Rev Lett 107(16) (2011) 166102). Here, we showed that molecular and mesoscale pictures agree by spatially averaging the dielectric constant obtained from molecular dynamics simulations over the distances relevant to the mean-field representation. In addition, the values of capacitances used to describe the electrical double layer in Surface Complexation Models (SCMs) of the mineral/electrolyte interface can be estimated using molecularly informed spatially averaged dielectric constants and positions of hydration layers. Experiments: First, we used molecular dynamics simulations to model the calcite 101¯4/electrolyte interface. Next, by using atomistic trajectories, we calculated the distance-dependent static dielectric constant and water density in the direction normal to the. Finally, we applied spatial compartmentalization consistent with the model of parallel-plate capacitors connected in series to estimate SCM capacitances. Findings: Computationally expensive simulations are required to determine the dielectric constant profile of interfacial water near the mineral surface. On the other hand, water density profiles are readily assessable from much shorter simulation trajectories. Our simulations confirmed that dielectric and water density oscillations at the interface are correlated. Here, we parametrized linear regression models to estimate the dielectric constant directly from the local water density. This is a significant computational shortcut compared to slowly converging calculations relying on total dipole moment fluctuations. The amplitude of the interfacial dielectric constant oscillation can exceed the dielectric constant of the bulk water, suggesting an ice-like frozen state, but only if there are no electrolyte ions. The interfacial accumulation of electrolyte ions causes a decrease in the dielectric constant due to the reduction of water density and re-orientation of water dipoles in ion hydration shells. Finally, we show how to use the computed dielectric properties to estimate SCM's capacitances.

58 GEOSCIENCES↗
NASA NTRS1990

Theory of plasma contactors in ground-based experiments and low Earth orbit

Previous theoretical work on plasma contactors as current collectors has fallen into two categories: collisionless double layer theory (describing space charge limited contactor clouds) and collisional quasineutral theory. Ground based experiments at low current are well explained by double layer theory, but this theory does not scale well to power generation by electrodynamic tethers in space, since very high anode potentials are needed to draw a substantial ambient electron current across the magnetic field in the absence of collisions (or effective collisions due to turbulence). Isotropic quasineutral models of contactor clouds, extending over a region where the effective collision frequency upsilon sub e exceeds the electron cyclotron frequency omega sub ce, have low anode potentials, but would collect very little ambient electron current, much less than the emitted ion current. A new model is presented, for an anisotropic contactor cloud oriented along the magnetic field, with upsilon sub e less than omega sub ce. The electron motion along the magnetic field is nearly collisionless, forming double layers in that direction, while across the magnetic field the electrons diffuse collisionally and the potential profile is determined by quasineutrality. Using a simplified expression for upsilon sub e due to ion acoustic turbulence, an analytic solution has been found for this model, which should be applicable to current collection in space. The anode potential is low and the collected ambient electron current can be several times the emitted ion current.

Gerver, M. J.↗
NASA NTRS1990

The impedance of a tubular electrode - A model for a porous electrode

A cylindrical tube is used as the basis for a two-dimensional mathematical model to calculate the impedance of a flooded porous electrode. The model incorporates charge-transfer, mass-transfer, and ohmic resistances to obtain the axial and radial dependencies of the concentration and potential profiles. A linearized Butler-Volmer kinetic expression for a simple redox reaction O + e yielding R is used, in conjuction with analytical expressions for the surface concentration and overpotential, to compute the open-circuit impedance. The results of the two-dimensional model, which omits double-layer charging, are compared with the results of a more standardly applied one-dimensional model in which radial variations are neglected, with and without double-layer charging. The simpler-to-apply one-dimensional model is found to be satisfactory when mass-transfer and ohmic resistances are small with respect to charge-transfer resistance. The omission of double-layer charging does not introduce error into the two-dimensional model in the frequency range in which capacitive-like effects are caused by mass-transfer limitations.

Viner, Andrew S.↗
DOE OSTI2020

Real-time mass spectrometric characterization of the solid–electrolyte interphase of a lithium-ion battery

Solid-electrolyte interphase (SEI) is a key component that dictates the performance of most electrochemical devices, but the understanding of its chemistry and structure has been limited by the lack of in-situ tools. In this work, we report SEI live-formation in Li-ion battery under operando condition with liquid secondary ion mass spectrometry (SIMS), which, in combination with molecular dynamics (MD) simulation, presents the first dynamic picture with molecular-accuracy about this key component. Before any interphasial chemistry occurs during the initial charging, an electric double layer forms at the electrode-electrolyte interface via the self-assembly of solvent molecules directed by both Li+ and potential of the electrified surface. Such double layer structure predicts the eventual interphasial chemistries formed from the electrolytes, where the negatively-charged electrode surface repels salt anions from the inner-Helmholtz layer and results in an inner SEI that is thin, dense and inorganic in nature but LiF-depleted. It was this dense layer that exercises the major functions of an interphase, i.e., conducting Li+ but insulating electrons. An outer layer that is electrolyte-permeable and organic-rich appears after formation of the inner SEI. In highly-concentrated electrolyte, the presence of LiF in the inner-SEI is raised due to the high population of salt anions in the double layer. These real-time observations at nano-scale reveal in general sense how an interphase inherits chemistry from inner-Helmholtz layer structure, and establish guidelines in engineering desirable interphases for the future battery chemistries.

Zhou, Yufan↗
DOE OSTI2018

Interface reconstruction with emerging charge ordering in hexagonal manganite

Multiferroic materials, which simultaneously have multiple orderings, hold promise for use in the next generation of memory devices. We report a novel self-assembled MnO double layer forming at the interface between a multiferroic YMnO 3 film and a c-Al 2 O 3 substrate. The crystal structures and the valence states of this MnO double layer were studied by atomically resolved scanning transmission electron microscopy and spectroscopy, as well as density functional theory (DFT) calculations. A new type of charge ordering has been identified within this MnO layer, which also contributes to a polarization along the [001] direction. DFT calculations further establish the occurrence of multiple couplings between charge and lattice in this novel double layer, in addition to the polarization in nearby YMnO 3 single layer. The interface reconstruction reported here creates a new playground for emergent physics, such as giant ferroelectricity and strong magnetoelectric coupling, in manganite systems.

36 MATERIALS SCIENCE↗
DOE OSTI2015

X-Ray Diffraction of Slag-Based Sodium Salt Waste Forms - 15513

Cementitious materials are used to solidify and stabilize aqueous based radioactive waste containing sodium salts. The types and proportions of cementitious ingredients used to treat aqueous radioactive waste streams containing sodium salts depend on the performance objectives for the waste forms and the compositions of the waste streams. This paper documents sample preparation and x-ray diffraction results for a series of materials made with water or highly alkaline sodium salt simulated waste water and cementitious binders. The objective of this study was to: 1) generate a base line for the evolution of the waste form as a function of time and conditions, 2) design new binders based on mineralogy of the binder, 3) understand and predict anion and cation leaching behavior of contaminants of concern, and 4) predict performance of the waste forms for which phase solubility and thermodynamic data are available. Characterization of the mineralogy is also important for understanding the buffering effects that the waste form has on infiltrating water / leachates. In summary, mixtures of Type II portland cement, Grade 100 ground granulated blast furnace slag (GGBFS) and carbon burn-out (CBO) Class F Fly ash which were hydrated with water contained hydrated phase assemblages typical of those reported in the literature. The calcium silicate hydrate phase assemblage in samples hydrated with the alkaline 4.4 M sodium salt simulated waste solution was found to be a function of the (CaO + MgO) / (SiO{sub 2} + Al{sub 2}O{sub 3}) ratio of the samples characterized. No significant differences were detected in samples cured 2 months and 14 months in sealed containers at ambient indoor temperatures. Slag and a blend of slag and cement hydrated with caustic 4.4 M Na salt solution resulted in the most crystalline matrix. In addition to poorly ordered C-S-H, these samples contained fairly well ordered C-S-H I (a precursor of 14A tobermorite) and 11 A Al-substituted tobermorite. These crystalline C-S-H phases did not form or were present in only trace amounts in slag blends containing about 45 to 62 mass percent fly ash. These slag-Class F fly ash blends had a higher silica plus alumina content relative to lime and magnesia than the blends that produced C-S-H I and Al-substituted tobermorite. The calcium silicate binder in the 10:45:45 mixture of cement: slag: fly ash was made up of poorly ordered C-S-H. The sample cured for 14 months may contain a small amount of the more crystalline calcium silicate hydrate phases. Layered double hydroxides in the hydrotalcite (magnesium-aluminum carbonate hydroxide) and hydrocalumite / AFm phases (calcium aluminum hydroxide) were present in mixtures containing slag. The specific phase(s) were not identified because these phases form solid solutions and have a considerable amount of overlap in their x-ray patterns. Sodium nitrate was the only sodium salt phase identified in x-ray diffraction patterns of the samples hydrated with salt solution. Drying during x-ray diffraction sample preparation may have resulted in precipitation of the sodium nitrate or it may have been present in the samples prior to x-ray sample preparation. Sodium sulfate, aluminate, and carbonate may have been incorporated in the structures of the layered double hydroxide (AFm) type phases. These mixed metal layered double hydroxides make up an important fraction of the matrix in the slag containing blends hydrated with caustic salt solution. They are among the few oxide-based phases that exhibit substantial, permanent anion exchange capacity [Kirkpatrick, et al. 1999, Plamer, et al., 2009, and Zhang and Reardon, 2003]. They also contribute to the structural properties of cementitious matrices [Taylor, 1997]. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Nonlinear low frequency electrostatic structures in a magnetized two-component auroral plasma

Finite amplitude nonlinear ion-acoustic solitons, double layers, and supersolitons in a magnetized two-component plasma composed of adiabatic warm ions fluid and energetic nonthermal electrons are studied by employing the Sagdeev pseudopotential technique and assuming the charge neutrality condition at equilibrium. The model generates supersoliton structures at supersonic Mach numbers regime in addition to solitons and double layers, whereas in the unmagnetized two-component plasma case only, soliton and double layer solutions can be obtained. Further investigation revealed that wave obliqueness plays a critical role for the evolution of supersoliton structures in magnetized two-component plasmas. In addition, the effect of ion temperature and nonthermal energetic electron tends to decrease the speed of oscillation of the nonlinear electrostatic structures. The present theoretical results are compared with Viking satellite observations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

The Effect of Proton Conductivity of Fe–N–C–Based Cathode on PEM Fuel cell Performance

A model–based impedance spectroscopy is used to determine proton conductivity, oxygen transport parameter, double layer capacitance and oxygen reduction reaction (ORR) Tafel slope in the Fe–N–C cathode catalyst layer (CCL) of a PEM fuel cell. Experimental spectra of two cells differing by the membrane thickness only are processed using a physics–based model for PEMFC impedance. The spectra have been measured in the range of current densities from 25 to 800 mA cm -2 . The ORR Tafel slope of both the cells shows almost linear growth with the current density. In one of the cells, the CCL proton conductivity σp strongly decays at the current density of 100 mA cm -2 ; this decay is accompanied by the step growth of the double layer capacitance. Other minor variations of proton conductivity and double layer capacitance with the cell current occur also in a counterphase; presumed origin of this effect is discussed. The oxygen diffusion coefficient in the cathode exhibits explosive growth with the cell current. We attribute this effect to formation of temperature and pressure gradients in the CCL due to strongly non–uniform distribution of ORR rate in the electrode.

25 ENERGY STORAGE↗
DOE OSTI2014

Double layer-like structures in the core of an argon helicon plasma source with uniform magnetic fields

A hot (T{sub e} ≈ 10 eV) electron population is observed in the core of a 3 mTorr argon helicon plasma source at 500 W RF power and 900 G uniform axial magnetic field strength, 12 cm from the edge of the helicon antenna. A double layer-like structure consisting of a localized axial electric field of approximately 8 V/cm over 1–2 cm is observed adjacent to the hot electron population. The potential step generated by the electric field is shown to be large enough to trap the hot electrons. To our knowledge this is the first observation of these structures in the core of a helicon discharge.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2019

Prediction of room-temperature half-metallicity in layered halide double perovskites

Half-metallic ferromagnets (HMFs) that possess intriguing physical properties with completely spin-polarized current are key candidates for high-efficiency spintronic devices. However, HMFs that could simultaneously have high Curie temperature ( T c ), wide half-metallic gap (Δ HM ), and large bulk magnetocrystalline anisotropy energy (MAE) are very rare, which significantly restrict their room-temperature (RT) applications. In this article, through materials screening in layered halide double perovskites (LHDPs), we have theoretically identified that Cs 4 FePb 2 Cl 12 , which has good crystallographic, dynamic and thermal stabilities, possesses an intrinsic half-metallic ground-state with a high T c ~ 450 K. Interestingly, the long-range ferromagnetic ordering in bulk Cs 4 FePb 2 Cl 12 is contributed by the strong super-superexchange interactions between the neighboring Fe d orbitals mediated by different anionic Cl p orbitals. The high T c of layered Cs 4 FePb 2 Cl 12 can be well maintained even in the monolayer limitation, i.e., T c ~ 370 K for Cs 4 FePb 2 Cl 12 monolayer, which is critical for nanoscale device applications. Moreover, both bulk and monolayer Cs 4 FePb 2 Cl 12 can exhibit wide Δ HM ~ 0.55 eV and large MAE >320 μeV/Fe, comparable to that of the best HMFs reported in the literature. Our findings can significantly extend the potentials of LHDPs for high-temperature spintronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Effective conductivity and permittivity of unsaturated porous materials in the frequency range 1 mHz-1GHz

A model combining low-frequency complex conductivity and high-frequency permittivity is developed in the frequency range from 1 mHz to 1 GHz. The low-frequency conductivity depends on pore water and surface conductivities. Surface conductivity is controlled by the electrical diffuse layer, the outer component of the electrical double layer coating the surface of the minerals. The frequency dependence of the effective quadrature conductivity shows three domains. Below a critical frequency f p , which depends on the dynamic pore throat size Λ, the quadrature conductivity is frequency dependent. Between f p and a second critical frequency f d , the quadrature conductivity is generally well described by a plateau when clay minerals are present in the material. Clay-free porous materials with a narrow grain size distribution are described by a Cole-Cole model. The characteristic frequency f d controls the transition between double layer polarization and the effect of the high-frequency permittivity of the material. The Maxwell-Wagner polarization is found to be relatively negligible. For a broad range of frequencies below 1 MHz, the effective permittivity exhibits a strong dependence with the cation exchange capacity and the specific surface area. At high frequency, above the critical frequency f d , the effective permittivity reaches a high-frequency asymptotic limit that is controlled by the two Archie’s exponents m and n like the low-frequency electrical conductivity. The unified model is compared with various data sets from the literature and is able to explain fairly well a broad number of observations with a very small number of textural and electrochemical parameters. It could be therefore used to interpret induced polarization, induction-based electromagnetic methods, and ground penetrating radar data to characterize the vadose zone.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1976

Electrostatic shocks as nonlinear ion acoustic waves

A cold fluid approach is presented which yields exact double-layer solutions that can be used to model electrostatic S-type shocks. Solutions derived from the two-temperature electron model are presented in order to show the range of amplitudes and scale lengths possible for this plasma model and to examine how shock properties depend on orientation of the shock. The dependence of various double-layer quantities on plasma composition is then considered for the cold electron beam model. Double-layer solutions pertinent to describing electrostatic shocks are pointed out.

Witt, E.↗
DOE OSTI2012

[La(UO{sub 2})V{sub 2}O{sub 7}][(UO{sub 2})(VO{sub 4})] the first lanthanum uranyl-vanadate with structure built from two types of sheets based upon the uranophane anion-topology

The new lanthanum uranyl vanadate divanadate, [La(UO{sub 2})V{sub 2}O{sub 7}][(UO{sub 2})(VO{sub 4})] was obtained by reaction at 800 Degree-Sign C between lanthanum chloride, uranium oxide (U{sub 3}O{sub 8}) and vanadium oxide (V{sub 2}O{sub 5}) and the structure was determined from single-crystal X-ray diffraction data. This compound crystallizes in the orthorhombic system with space group P2{sub 1}2{sub 1}2{sub 1} and unit-cell parameters a=6.9470(2) A, b=7.0934(2) A, c=25.7464(6) A, V=1268.73(5) A{sup 3}, Z=4. A full matrix least-squares refinement yielded R{sub 1}=0.0219 for 5493 independent reflections. The crystal structure is characterized by the stacking of uranophane-type sheets {sup 2}{sub {infinity}}[(UO{sub 2})(VO{sub 4})]{sup -} and double layers {sup 2}{sub {infinity}}[La(UO{sub 2})(V{sub 2}O{sub 7})]{sup +} connected through La-O bonds involving the uranyl oxygen of the uranyl-vanadate sheets. The double layers result from the connection of two {sup 2}{sub {infinity}}[La(UO{sub 2})(VO{sub 4}){sub 2}]{sup -} sheets derived from the uranophane anion-topology by replacing half of the uranyl ions by lanthanum atoms and connected through the formation of divanadate entities. - Graphical abstract: A view of the three-dimensional structure of [La(UO{sub 2})V{sub 2}O{sub 7}][(UO{sub 2})(VO{sub 4})]. Highlights: Black-Right-Pointing-Pointer New lanthanum uranyl vanadate divanadate has been synthesized. Black-Right-Pointing-Pointer Structure was determined from single-crystal X-ray diffraction data. Black-Right-Pointing-Pointer Structure is characterized by uranophane-type sheets and double layers {sup 2}{sub {infinity}}[La(UO{sub 2})(V{sub 2}O{sub 7})]{sup +}.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

On the hysteresis in fireball formation and extinction

A model is proposed to explain hysteresis observed in reball formation and extinction as electrode bias is varied in partially ionized plasmas. Formation is predicted after a su ciently deep potential well for electrons is established in the electron sheath of the electrode. Under the experimental conditions considered, once the reball forms the plasma potential rapidly increases, resulting in electrons being only lost to the electrode.Previous predictions suggest that once formed the reball double layer must maintain a potential close to the ionization potential of the neutral gas to remain in a steady state. In this paper, it is predicted that changes in electrode bias after formation results in a corresponding change in reball size and plasma potential. This change in plasma potential allows the double layer potential to be maintained at biases both above and below the electrode bias at onset. The reball extinguishes when the required double layer potential can no longer be maintained with balance of current loss of the bulk plasma. These predictions are tested experimentally and are found to be in good agreement with the measurements.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1992

The scaling of relativistic double-year widths - Poisson-Vlasov solutions and particle-in-cell simulations

The study of relativistic plasma double layers is described through the solution of the one-dimensional, unmagnetized, steady-state Poisson-Vlasov equations and by means of one-dimensional, unmagnetized, particle-in-cell simulations. The thickness vs potential-drop scaling law is extended to relativistic potential drops and relativistic plasma temperatures. The transition in the scaling law for 'strong' double layers suggested by analytical two-beam models by Carlqvist (1982) is confirmed, and causality problems of standard double-layer simulation techniques applied to relativistic plasma systems are discussed.

Sulkanen, Martin E.↗