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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2012

Thickness measurements of nanoscale brine films on silica surfaces under geologic CO 2 sequestration conditions using synchrotron X-ray fluorescence

In reservoirs used for geologic CO 2 sequestration, brine films remaining on mineral surfaces can influence flow, diffusion, and reactions. We have examined how the capillary (disjoining) potential influences the thickness of a KCsI 2 brine film on both smooth and rough SiO 2 surfaces [root mean square roughness (Rrms), 1.6 and 330 nm, respectively], under confinement with supercritical (sc) CO2. The thicknesses of brine films coating interior surfaces of SiO 2 windows in a high-pressure cell were determined through synchrotron X-ray fluorescence of two tracer ions (I - and Cs +) at 7.8 MPa and 40°C (representative of conditions at about 0.78 km below the land surface), with scCO 2 as the immiscible confining fluid. The measured area-averaged film thicknesses on the 330 nm Rrms silica surface ranged from 265 to 249 nm for capillary potentials measured within a narrow range from 0.18 to 3.7 kPa. Over this same range of potentials, film thicknesses measured on the smooth (1.6 nm Rrms) silica surface were about 2 nm, although equilibrium does not seem to have been achieved. The measured average brine film thicknesses were critically controlled by surface roughness, with very weak variation in response to the fairly narrow range of tested capillary potentials.

58 GEOSCIENCES↗
DOE OSTI2015

Stability of Surface and Subsurface Hydrogen on and in Au/Ni Near-Surface Alloys

Periodic, self-consistent DFT-GGA (PW91) calculations were used to study the interaction of hydrogen atoms with the (111) surfaces of substitutional near-surface alloys (NSAs) of Au and Ni with different surface layer compositions and different arrangements of Au atoms in the surface layer. The effect of hydrogen adsorption on the surface and in the first and second subsurface layers of the NSAs was studied. Increasing the Au content in the surface layer weakens hydrogen binding on the surface, but strengthens subsurface binding, suggesting that the distribution of surface and subsurface hydrogen will be different than that on pure Ni(111). While the metal composition of the surface layer has an effect on the binding energy of hydrogen on NSA surfaces, the local composition of the binding site has a stronger effect. For example, fcc hollow sites consisting of three Ni atoms bind H nearly as strongly as on Ni(111), and fcc sites consisting of three Au atoms bind H nearly as weakly as on Au(111). Sites with one or two Au atoms show intermediate binding energies. The preference of hydrogen for three-fold Ni hollow sites alters the relative stabilities of different surface metal atom arrangements, and may provide a driving force for adsorbate-induced surface rearrangement.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2021

Reducing Surface Recombination Velocity of Methylammonium-Free Mixed-Cation Mixed-Halide Perovskites via Surface Passivation

We control surface recombination in the mixed-cation, mixed-halide perovskite, FA0.83Cs0.17Pb(I0.85Br0.15)3, by passivating nonradiative defects with the polymerizable Lewis base (3-aminopropyl)trimethoxysilane (APTMS). We demonstrate average minority carrier lifetimes >4 µs, nearly single exponential monomolecular photoluminescence decays, and high external photoluminescence quantum efficiencies (>20%, corresponding to ~97% of the maximum theoretical quasi-Fermi-level splitting) at low excitation fluence. We confirm both the composition and valence band edge position of the FA0.83Cs0.17Pb(I0.85Br0.15)3 perovskite using multi-institutional, cross-validated, X-ray photoelectron spectroscopy and UV photoelectron spectroscopy measurements. We extend the APTMS surface passivation to higher bandgap double-cation (FA and Cs) compositions (1.7, 1.75, and 1.8 eV) as well as the widely used triple-cation (FA, MA, and Cs) composition. Finally, we demonstrate that the average surface recombination velocity decreases from ~1000 to ~10 cm/s post APTMS passivation for FA0.83Cs0.17Pb(I0.85Br0.15)3. Our results demonstrate that surface-mediated recombination is the primary nonradiative loss pathway in many methylammonium (MA)-free mixed-cation mixed-halide films with a range of different bandgaps, which is a problem observed for a wide range of perovskite active layers and reactive electrical contacts. Our study also provides insights to develop passivating molecules that help reduce surface recombination in MA-free mixed-cation mixed-halide films and indicates that surface passivation and contact engineering will enable near-theoretical device efficiencies with these materials.

14 SOLAR ENERGY↗
DOE OSTI2018

CAUSES: On the Role of Surface Energy Budget Errors to the Warm Surface Air Temperature Error Over the Central United States

Many weather forecasting and climate models simulate a warm surface air temperature (T2m) bias over mid-latitude continents during the summertime, especially over the Great Plains. We present here one of a series of papers from a multi-model intercomparison project (CAUSES: Cloud Above the United States and Errors at the Surface), which aims to evaluate the role of cloud, radiation, and precipitation biases in contributing to T2m bias using a short-term hindcast approach with observations mainly from the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site during the period of April to August 2011. The present study examines the contribution of surface energy budget errors to the bias. All participating models simulate higher net shortwave and longwave radiative fluxes at the surface but there is no consistency on signs of biases in latent and sensible heat fluxes over the Central U.S. and ARM SGP. Nevertheless, biases in net shortwave and downward longwave fluxes, as well as surface evaporative fraction (EF) are the main contributors to T2m bias. Radiation biases are largely affected by cloud simulations, while EF is affected by soil moisture modulated by seasonal accumulated precipitation and evaporation. An approximate equation is derived to further quantify the magnitudes of radiation and EF contributions to T2m bias. Our analysis suggests that radiation errors are always an important source of T2m error for long-term climate runs with EF errors either of equal or lesser importance. However, for the short-term hindcasts, EF errors are more important provided a model has a substantial EF bias.

Ma, H. -Y.↗
DOE OSTI2016

Impacts of Surface Site Coordination on Arsenate Adsorption: Macroscopic Uptake and Binding Mechanisms on Aluminum Hydroxide Surfaces

Aluminum hydroxides play important roles in regulating the fate and transport of contaminants and nutrients in soils and aquatic systems. Like many metal oxides, these minerals display surface functional groups in a series of coordination states, each of which may differ in its affinity for adsorbates. The distribution of functional group types varies among distinct surfaces of aluminum hydroxides, and we thus hypothesize that the adsorption behavior and mechanisms will show a dependence on particle morphology. To test this hypothesis, we investigate arsenate adsorption on two aluminum hydroxide polymorphs with distinct particle morphologies, gibbsite [γ-Al(OH) 3 ] and bayerite [α-Al(OH) 3 ], at pH 4 and 7. Synthetic gibbsite platelets expose large (001) basal surfaces predicted to be terminated by doubly coordinated functional groups (>Al 2 OH). In contrast, synthetic bayerite microrods display mainly edge surfaces (parallel to the c axis) containing abundant singly coordinated functional groups (>AlOH 2 ). Macroscopic adsorption studies show that gibbsite adsorbs less arsenate per unit surface area than bayerite at both pH values and suggest that two surface complexes form on each material. Similar electrokinetic behavior is displayed at the same relative coverages of arsenate, suggesting that similar reactive surface groups (>AlOH 2 ) control the surface charging on both particles. EXAFS spectroscopy shows that there is no variation in arsenate surface speciation on a given mineral with surface coverage or pH. Whereas bidentate binuclear inner-sphere species are the dominant complexes present, the EXAFS result suggest that outer-sphere species also occur on both minerals, with a greater abundance on gibbsite. This binding mode likely involves adsorption to >Al 2 OH sites, which have a slow ligand exchange rate that inhibits inner-sphere binding. Lastly, these results demonstrate that adsorption mechanisms and capacity, even when normalized for specific surface area, vary with metal oxide particle morphology because of the distribution of distinct functional groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Surface degradation of Li{sub 1–x}Ni{sub 0.80}Co{sub 0.15}Al{sub 0.05}O{sub 2} cathodes: Correlating charge transfer impedance with surface phase transformations

The pronounced capacity fade in Ni-rich layered oxide lithium ion battery cathodes observed when cycling above 4.1 V (versus Li/Li{sup +}) is associated with a rise in impedance, which is thought to be due to either bulk structural fatigue or surface reactions with the electrolyte (or combination of both). Here, we examine the surface reactions at electrochemically stressed Li{sub 1–x}Ni{sub 0.8}Co{sub 0.15}Al{sub 0.05}O{sub 2} binder-free powder electrodes with a combination of electrochemical impedance spectroscopy, spatially resolving electron microscopy, and spatially averaging X-ray spectroscopy techniques. We circumvent issues associated with cycling by holding our electrodes at high states of charge (4.1 V, 4.5 V, and 4.75 V) for extended periods and correlate charge-transfer impedance rises observed at high voltages with surface modifications retained in the discharged state (2.7 V). The surface modifications involve significant cation migration (and disorder) along with Ni and Co reduction, and can occur even in the absence of significant Li{sub 2}CO{sub 3} and LiF. These data provide evidence that surface oxygen loss at the highest levels of Li{sup +} extraction is driving the rise in impedance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Variations of ionization potential and electron affinity as a function of surface orientation: The case of orthorhombic SnS

We investigated the dependence of absolute SnS band-edge energies on surface orientation using density functional theory and GW method for all surfaces with Miller indices $-3 ≤ h,k,l ≤ 3$ and found variations as large as 0.9 eV as a function of ($hkl$). Variations of this magnitude may affect significantly the performance of photovoltaic devices based on polycrystalline SnS thin-films and, in particular, may contribute to the relatively low measured open circuit voltage of SnS solar cells. X-ray diffraction measurements confirm that our thermally evaporated SnS films exhibit a wide distribution of different grain orientations, and the results of Kelvin force microscopy support the theoretically predicted variations of the absolute band-edge energies.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Anomalous grain growth in the surface region of a nanocrystalline CeO2 film under low-temperature heavy ion irradiation

Grain growth and phase stability of nanocrystalline ceria are investigated under ion irradiation at different temperatures. Irradiations at temperatures of 300 and 400 K result in uniform grain growth throughout the film. Anomalous grain growth is observed in thin films of nanocrystalline ceria under 3 MeV Au+ irradiation at 160 K. At this low temperature, significant grain growth is observed within 100 nm from the surface, no obvious growth is detected in the rest of the films. While the grain growth is attributed to a defect-stimulated mechanism at room temperature and above, a defect diffusion-limited mechanism is significant at low temperature with the primary defect responsible being the oxygen vacancy. The nanocrystalline grains remain in the cubic phase regardless of defect kinetics.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2012

Identification of Simultaneous U(VI) Sorption Complexes and U(IV) Nanoprecipitates on the Magnetite (111) Surface

Sequestration of uranium (U) by magnetite is a potentially important sink for U in natural and contaminated environments. However, molecular-scale controls that favor U(VI) uptake including both adsorption of U(VI) and reduction to U(IV) by magnetite remain poorly understood, in particular, the role of U(VI)-CO{sub 3}-Ca complexes in inhibiting U(VI) reduction. To investigate U uptake pathways on magnetite as a function of U(VI) aqueous speciation, we performed batch sorption experiments on (111) surfaces of natural single crystals under a range of solution conditions (pH 5 and 10; 0.1 mM U(VI); 1 mM NaNO{sub 3}; and with or without 0.5 mM CO{sub 3} and 0.1 mM Ca) and characterized surface-associated U using grazing incidence extended X-ray absorption fine structure spectroscopy (GI-EXAFS), grazing incidence X-ray diffraction (GI-XRD), and scanning electron microscopy (SEM). In the absence of both carbonate ([CO{sub 3}]T, denoted here as CO{sub 3}) and calcium (Ca), or in the presence of CO{sub 3} only, coexisting adsorption of U(VI) surface species and reduction to U(IV) occurs at both pH 5 and 10. In the presence of both Ca and CO{sub 3}, only U(VI) adsorption (VI) occurs. When U reduction occurs, nanoparticulate UO{sub 2} forms only within and adjacent to surface microtopographic features such as crystal boundaries and cracks. This result suggests that U reduction is limited to defect-rich surface regions. Further, at both pH 5 and 10 in the presence of both CO{sub 3} and Ca, U(VI)-CO{sub 3}-Ca ternary surface species develop and U reduction is inhibited. These findings extend the range of conditions under which U(VI)-CO{sub 3}-Ca complexes inhibit U reduction.

99 GENERAL AND MISCELLANEOUS↗