Pre‐Industrial, Present and Future Atmospheric Soluble Iron Deposition and the Role of Aerosol Acidity and Oxalate Under CMIP6 Emissions
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Elisa Bergas‐Massó↗
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Apparent Enhanced Solubility of Single‐Wall Carbon Nanotubes in a Deuterated Acid Mixture
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T. Ramanathan↗
Model simulations of rainout and washout from a warm stratiform cloud
A one-dimensional, time-dependent cloud model with parameterized microphysics is used to investigate the processes which control the rainout and washout of soluble gases from warm, precipitating stratiform clouds. Calculations are presented simulating the distributions of soluble species within and below the cloud layer and in the precipitating raindrops as a function of time and species' solubility. Calculations indicate that for species with low solubility, wet removal processes are relatively slow and thus do not significantly affect the species' gas-phase abundance. As a result, the removal of low-solubility species by rainout and washout is controlled by thermodynamic processes with the concentration of the species in cloud and rainwater largely determined by the species' solubility. For highly soluble species on the other hand, dissolution into cloud droplets and removal in rain is quite rapid and the abundance of highly soluble species within and below the cloud falls rapidly as soon as the precipitation begins.
Xing, Lin↗
Core-Mantle Fractionation of Carbon in Earth and Mars: the Effects of Sulfur
Constraining carbon (C) fractionation between silicate magma ocean (MO) and core-forming alloy liquid during early differentiation is essential to understand the origin and early distribution of C between reservoirs such as the crust-atmosphere, mantle, and core of Earth and other terrestrial planets. Yet experimental data at high pressure (P)-temperature (T) on the effect of other light elements such as sulfur (S) in alloy liquid on alloy-silicate partitioning of C and C solubility in Fe-alloy compositions relevant for core formation is lacking. Here we have performed multi-anvil experiments at 6–13 GPa and 1800–2000 °C to examine the effects of S and Ni on the solubility limit of C in Fe-rich alloy liquid as well as partitioning behavior of C between alloy liquid and silicate melt (𝐷𝐷(sub C)(sup alloy/silicate)). The results show that C solubility in the alloy liquid as well as 𝐷𝐷(sub C)(sup alloy/silicate) decreases with increasing in S content in the alloy liquid. Empirical regression on C solubility in alloy liquid using our new experimental data and previous experiments demonstrates that C solubility significantly increases with increasing temperature, whereas unlike in S-poor or S-free alloy compositions, there is no discernible effect of Ni on C solubility in S-rich alloy liquid. Our modelling results confirm previous findings that in order to satisfy the C budget of BSE, the bulk Earth C undergoing alloy-silicate fractionation needs to be as high as those of CI-type carbonaceous chondrite, i.e., not leaving any room for volatility-induced loss of carbon during accretion. For Mars, on the other hand, an average single-stage core formation at relatively oxidized conditions (1.0 log unit below IW buffer) with 10-16 wt.% S in the core could yield a Martian mantle with a C budget similar to that of Earth’s BSE for a bulk C content of ~0.25-0.9 wt.%. For the scenario where C was delivered to the proto-Earth by a S-rich differentiated impactor at a later stage, our model calculations predict that bulk C content in the impactor can be as low as ~0.5 wt.% for an impactor mass that lies between 9-20% of present day Earth’s mass. This value is much higher than 0.05-0.1 wt.% bulk C in the impactor predicted by Li et al. (2016) because C-solubility limit of 0.3 wt.% in a S-rich alloy predicted by their models is significantly lower than the experimentally derived C-solubility of ~1.6 wt. % for the relevant S-content in the core of the impactor.
Carbon↗
Experimental constraints on CO2 and H2O in the Martian mantle and primary magmas
We present new data on the stability of hornblende in a Martian mantle composition, on CO2 solubility in iron-rich basaltic magmas, and on the solubility of H2O in an alkalic basaltic magma. These new data are combined with a summary of data from the literature to present a summary of the current state of our estimates of solubilities of H2O and CO2 in probable Martian magmas and the stability of hornblende in a slightly hydrous mantle. The new results suggest that hornblende stability is not sensitive to the Mg/(Mg+Fe) ratio (mg#) of the mantle, that is the results for terrestrial mantle compositions are similar to the more iron-rich Martian composition. Likewise, CO2 solubility in iron-rich tholeiitic basaltic magmas is similar to iron-poor terrestrial compositions. The solubility of H2O has been measured in an alkalic basaltic (basanite) composition for the first time, and it is significantly lower than predicted for models of water solubility in magmas. The lack of mg# dependence observed in hornblende stability and on CO2 solubility that in many cases terrestrial results can be applied to Martian compositions. This conclusion does not apply to other phenomena such as primary magma compositions and major mantle mineral mineralogy.
Holloway, John R.↗
Sulfur Saturation Limits in Silicate Melts and their Implications for Core Formation Scenarios for Terrestrial Planets
This study explores the controls of temperature, pressure, and silicate melt composition on S solubility in silicate liquids. The solubility of S in FeO-containing silicate melts in equilibrium with metal sulfide increases significantly with increasing temperature but decreases with increasing pressure. The silicate melt structure also exercises a control on S solubility. Increasing the degree of polymerization of the silicate melt structure lowers the S solubility in the silicate liquid. The new set of experimental data is used to expand the model of Mavrogenes and O'Neill(1999) for S solubility in silicate liquids by incorporating the influence of the silicate melt structure. The expected S solubility in the ascending magma is calculated using the expanded model. Because the negative pressure dependence of S solubility is more influential than the positive temperature dependence, decompression and adiabatic ascent of a formerly S-saturated silicate magma will lead to S undersaturation. A primitive magma that is S-saturated in its source region will, therefore, become S-undersaturated as it ascends to shallower depth. In order to precipitate magmatic sulfides, the magma must first cool and undergo fractional crystallization to reach S saturation. The S content in a metallic liquid that is in equilibrium with a magma ocean that contains approx. 200 ppm S (i.e., Earth's bulk mantle S content) ranges from 5.5 to 12 wt% S. This range of S values encompasses the amount of S (9 to 12 wt%) that would be present in the outer core if S is the light element. Thus, the Earth's proto-mantle could be in equilibrium (in terms of the preserved S abundance) with a core-forming metallic phase.
Holzheid, Astrid↗
Carbon, hydrogen and nitrogen isotopes in solvent-extractable organic matter from carbonaceous chondrites
CCl4 and CH3OH solvent extractions were performed on the Murray, Murchison, Orgueil and Renazzo carbonaceous chondrites. Delta-D values of +300-+500% are found in the case of the CH3OH-soluble organic matter. The combined C, H and N isotope data makes it unlikely that the CH3OH-soluble components are derivable from, or simply related to, the insoluble organic polymer found in the same meteorites. A relation between the event that formed hydrous minerals in CI1 and CM2 meteorites and the introduction of water- and methanol-soluble organic compounds is suggested. Organic matter soluble in CCl4 has no N, and delta-C-13 values are lower than for CH3OH-soluble phases. It is concluded that there either are large isotopic fractionations for carbon and hydrogen between different soluble organic phases, or the less polar components are partially of terrestrial origin.
Becker, R. H.↗
Comment on 'Summary and implications of reported amino acid concentrations in the Murchison meteorite' by E. L. Shock and M. D. Schulte
A criticism of the claim by Shock and Schulte (1990) that there is a correlation between the amino acid abundances (relative to glycine) in the Murchison meteorite and their aqueous solubilities is presented. Their suggestion that 'the same factors which control the aqueous solubility of many amino acids also control their relative abundances in the Murchison meteorite is argued to be incorrect. It is proposed that even though the water/meteorite ratio would have been less during meteorite aqueous alteration than that in the 100-C laboratory extraction procedure, amino acids are simply too soluble. The distribution of other meteorite organic components such as PAHs may have been affected by alteration because they are only slightly soluble in water and can be easily separated by geochromatographic processes. In their reply Shock and Schulte contend that the critics argue against a point not made in their paper and that their argument was supported with several unsubstantiated assertions, including an unfounded claim that the temperature dependence of amino acid solubilities are 'not greatly different', a misrepresentation of isopiestic studies on concentration solutions as equilibrium solubility measurements.
Miller, Stanley L.↗
Methanol Uptake by Low Temperature Aqueous Sulfuric Acid Solutions
The global methanol budget is currently unbalanced, with source terms significantly larger than the sinks terms. To evaluate possible losses of gaseous methanol to sulfate aerosols, the solubility and reactivity of methanol in aqueous sulfuric acid solutions representative of upper tropospheric and lower stratospheric aerosols is under investigation. Methanol will partition into sulfate aerosols according to its Henry's law solubility. Using standard uptake techniques in a Knudsen cell reactor, we have measured the effective Henry's law coefficient, H*, for cold (196 - 220 K) solutions ranging between 45 and 70 wt % H2SO4. We have found that methanol solubility ranges from approx. 10(exp 5) - 10(exp 7) M/atm for UT/LS conditions. Solubility increases with decreasing temperature and with increasing sulfuric acid content. Although methanol is slightly more soluble than are acetone and formaldehyde, current data indicate that uptake by clean aqueous sulfuric acid particles will not be a significant sink for methanol in the UT/LS. These solubility measurements include uptake due to physical solvation and any rapid equilibria which are established in solution. Reaction between primary alcohols and sulfuric acid does occur, leading to the production of alkyl sulfates. Literature values for the rate of this reaction suggest that formation of CH3OSO3H is not significant over our experimental time scale for solutions below 80 wt % H2SO4. To confirm this directly, results obtained using a complementary equilibrium measurement technique will also be presented.
Iraci, L. T.↗
Organic Analysis in the Miller Range 090657 CR2 Chondrite: Part 2 Amino Acid Analyses
Primitive carbonaceous chondrites contain a wide variety of organic material, ranging from soluble discrete molecules to insoluble, unstructured kerogen-like components, as well as structured nano-globules of macromolecular carbon. The relationship between the soluble organic molecules, macromolecular organic material, and host minerals are poorly understood. Due to the differences in extractability of soluble and insoluble organic materials, the analysis methods for each differ and are often performed independently. The combination of soluble and insoluble analyses, when performed concurrently, can provide a wider understanding of spatial distribution, and elemental, structural and isotopic composition of organic material in primitive meteorites. Using macroscale extraction and analysis techniques in combination with in situ microscale observation, we have been studying both insoluble and soluble organic material in the primitive CR2 chondrite Miller Range (MIL) 090657. In accompanying abstracts (Cao et al. and Messenger et al.) we discuss insoluble organic material in the samples. By performing the consortium studies, we aim to improve our understanding of the relationship between the meteorite minerals and the soluble and insoluble organic phases and to delineate which species formed within the meteorite and those that formed in nebular or presolar environments. In this abstract, we present the results of amino acid analyses of MIL 090657 by ultra performance liquid chromatography with fluorescence detection and quadrupole-time of flight mass spectrometry. Amino acids are of interest because they are essential to life on Earth, and because they are present in sufficient structural, enantiomeric and isotopic diversity to allow insights into early solar system chemical processes. Furthermore, these are among the most isotopically anomalous species, yet at least some fraction are thought to have formed by aqueously-mediated processes during parent body alteration.
Burton, A. S.↗
Cycling phosphorus on the Archean Earth: Part II. Phosphorus limitation on primary production in Archean ecosystems
Several lines of evidence point to low rates of net primary production (NPP) in Archean oceans. However, whether Archean NPP was limited by electron donors or nutrients, particularly phosphorus (P), and how these factors might have changed over a billion years of recorded Archean history, remains contentious. One major challenge is to understand quantitatively the biogeochemical cycling of P on the early Earth. In Part I of this series (Hao et al., 2020), we estimated the weathering flux of P to the oceans as a function of temporally increasing continental emergence and elevation through Archean time. In Part II, we conduct thermodynamic and kinetic simulations to understand key processes of P cycling within the Archean ocean, including seafloor weathering, recycling of organic P, the solubility and precipitation of secondary phosphate minerals, and the burial diagenesis of P precipitates. Our calculations suggest low solubilities of apatite minerals in Archean seawater, primarily due to nearly neutral pH and high levels of Ca. This low solubility, in turn, implies a negligible contribution of apatite dissolution to P bioavailability in Archean seawater. We also simulate the solubility limits of common secondary P-bearing minerals, showing that vivianite would have been the least soluble P mineral in ferruginous Archean seawater (0.1–0.3 µM), even at moderate supersaturation states (Ω = 100 or 1000). If vivianite precipitation was kinetically favorable by microbial activities and mineral adsorption, the sinking flux of P as vivianite in Archean seawater could have reached the modern sinking flux, implying that vivianite precipitation was a potentially major sink for P in Archean oceans. During burial diagenesis, however, vivianite in porewater would have become less stable than Ca-phosphates of lower solubility. At elevated temperatures (>100 °C) associated with burial diagenesis and low-grade metamorphism, vivianite is predicted to react irreversibly with calcite to form apatite. Optimistic assumptions about the recycling efficiency of P on the Archean Earth lead us to estimate that by the end of the eon the total flux of P (continental weathering + recycling) could have supported NPP at levels up to 7% of the modern. The total flux of P would have been much lower on the early and middle Archean Earth, whereas fluxes of electron donors could have been higher, suggesting very low productivity and P-limitation of marine ecosystems during much of the eon. Comparing our estimates of NPP as limited by P supply with the estimate by Ward et al. (2019), in which NPP was limited by electron donors and metabolic efficiency, there could have been a transition between P-limited productivity in the early to middle Archean to electron donor-limitation closer to the eon’s end (assuming no oxygenic photosynthesis). Once oxygenic photosynthesis reached ecological significance, probably near the end of the Archean, our estimated flux of P would allow rapid oxidation of atmosphere.
Vivianite↗
In-flight and laboratory vacuum-friction test results
Coefficient of friction measurements were made for six unlubricated metal couples exposed to the space environment aboard the OV-1-13 spacecraft and exposed to laboratory vacuum. Materials studied included mutually soluble, partially soluble, and insoluble metal combinations. Two samples of each material couple were tested in space and in the laboratory using the disk and rider technique. Linear velocity was 0.10 cm/s (2.5 in/min) and rider normal load was 4.45 N (1 lb) for the gold versus silver couples and 8.90 N (2lb) for the other combinations. Results showed that friction data obtained in a clean ion-pumped laboratory vacuum of 10 to the minus 10 power materials with low mutual solubility can be correlated to operation in the vicinity of a typical scientific spacecraft that is exposed to an ambient pressure as low as 10 to the minus 12 power torr. The expected increase in coefficient of friction with solubility was shown. Material couples with high mutual solubility present the hazard of unpredictable drastic friction increase in orbit which may not be evident in laboratory testing at levels down to 10 to the minus 10 power torr. It was also shown that gross cold welding of unlubricated metals exposed to a satellite environment does not occur.
Devine, E. J.↗
A simple approach to metal hydride alloy optimization
Hildebrand-Scott (1950) solubility parameters can be obtained for metals and alloys by calculating the cohesive energy density (CED), equal to the square of the solubility parameter, and a function of the heat of sublimation and the atomic volume. It is suggested that the solubility parameter permits estimation of the hydrogen storage capacity of an alloy and that alloys with a solubility parameter approximately equal to the parameter for hydrogen will have greater hydrogen storage capacity than other alloys. Equilibrium pressure - temperature relationships for some metal hydrides are presented in conjunction with the calculated solubility parameter and correlated with characteristics which would be useful in hydrogen-powered vehicles. Alloy properties which increase the amount of nonstoichiometric reversible hydrogen absorption are discussed.
Lawson, D. D.↗
Aspects of the history of 66095 based on trace elements in clasts and whole rock
Halogens, P, U and Na are reported in anorthositic and basaltic clasts and matrix from rusty rock 66095. Large fractions of Cl and Br associated with the separated phases from 66095 are soluble in H2O. Up to two orders of magnitude variation in concentrations of these elements in the breccia components and varying H2O-soluble Cl/Br ratios indicate different sources of volatiles. An approximately constant ratio of the H2O- to 0.1 M HNO3-soluble Br in the various components suggests no appreciable alteration in the original distributions of this element in the breccia forming processes. Up to 50% or more of the phosphorus and of the non-H2O-soluble Cl was dissolved from most of the breccia components by 0.1 M HNO3. Clast and matrix residues from the leaching steps contain, in most cases, the Cl/P2O5 ratio found in 66095 whole rock and in a number of other Apollo 16 samples. Evidence that phosphates are the major P-phases in the breccia is based on the 0.1 M acid solubility of Cl and P in the matrix sample and on elemental concentrations which are consistent with those of KREEP.
Jovanovic, S.↗
Property enchancement of polyimide films by way of the incorporation of lanthanide metal ions
Lanthanide metal ions were incorporated into the polyimide derived from 2,2-bis(3,4-dicarboxyphenyl) hexafluoropropane dianhydride (6FDA) and 1,3-bis(aminophenoxy) benzene (APB) in an attempt to produce molecular level metal-polymer composites. The lanthanide series of metal ions (including aluminum, scandium, and yttrium) provide discrete and stable metal ions in the 3+ oxidation state. Throughout the series there is a uniform variation in ionic size ranging from 50 pm for aluminum to a maximum of 103.4 pm for cerium and gradually decreasing again to 84.8 pm for lutetium. The high charge-to-size ratio for these ions as well as the ability to obtain large coordination numbers makes them excellent candidates for interacting with the polymer substructure. The distinct lack of solubility of simple lanthanide salts such as the acetates and halides has made it difficult to obtain metal ions distributed in the polymer framework as discrete ions or metal complexes rather than microcomposites of metal clusters. (Lanthanum nitrates are quite soluble, but the presence of the strongly oxidizing nitrate ion leads to serious degradation of the polymer upon thermal curing. This work was successful at extending the range of soluble metals salts by using chelating agents derived from the beta-diketones dipivaloylmethane, dibenzoylmethane, trifluoroacetylacetone, and hexafluoroacetylacetone. Metal acetates which are insoluble in dimethylacetamide dissolve readily in the presence of the diketones. Addition of the polyimide yields a homogeneous resin which is then cast into a clear film. Upon curing clear films were obtained with the dibenzoylmethane and trifluoroacetylacetone ligands. The dipavaloylmethane precipitates the metal during the film casting process, and hexafluoroacetylacetone gives cured films which are deformed and brittle. These clear films are being evaluated for the effect of the metal ions on the coefficient of thermal expansion, resistance to atomic oxygen, and on selective gas permeability. Much more commonly than above, polyimide films are prepared by casting the film as the poly(amic acid) precursor which is then converted to the imidized form during the thermal cure cycle. Very limited success was achieved in the past in adding lanthanide metal ions to the amide precursors because of gellation and lack of solubility. With the use of the diketone ligands cited above, the solubility and gellation problems were overcome. However, the films after curing were clear but unacceptably brittle. Attempts to overcome this cure embrittlement problem are in progress.
Thompson, David W.↗
The pH of Mars
The Viking labeled release (LR) experiments provided data that can be used to determine the acid-base characteristics of the regolith. Constraints on the acid-base properties and redox potentials of the Martian surface material would provide additional information for determining what reactions are possible and defining formation conditions for the regolith. Calculations devised to determine the pH of Mars must include the amount of soluble acid species or base species present in the LR regolith sample and the solubility product of the carbonate with the limiting solubility. This analysis shows that CaCO3, either as calcite or aragonite, has the correct K(sub sp) to have produced the Viking LR successive injection reabsorption effects. Thus CaCO3 or another MeCO3 with very similar solubility characteristics must have been present on Mars. A small amount of soluble acid, but no more than 4 micro-mol per sample, could also have been present. It is concluded that the pH of the regolith is 7.2 +/- 0.1.
Plumb, R. C.↗
Synthesis and Characterization of High Performance Polyimides Containing the Bicyclo(2.2.2)oct-7-ene Ring System
Due to the difficulty in processing polyimides with high temperature stability and good solvent resistance, we have synthesized high performance polyimides with bicyclo(2.2.2)-oct-7-ene ring system which can easily be fabricated into films and fibers and subsequently converted to the more stable aromatic polyimides. In order to improve processability, we prepared two polyimides by reacting 1,4-phenylenediamine and 1,3phenylediamine with bicyclo(2.2.2)-7-octene-2,3,5,6-tetracarboxylic dianhydride. The polyimides were characterized by FTIR, FTNMR, solubility and thermal analysis. Thermogravimetric analysis (TGA) showed that the 1,4-phenylenediamine and 1,3-phenylenediamine containing polyimides were stable up to 460 and 379 C, respectively under nitrogen atmosphere. No melting transitions were observed for both polyimides. The 1,4-phenylenediamine containing polyimide is partially soluble in dimethyl sulfoxide, methane sulfonic acid and soluble in sulfuric acid at room temperature. The 1,3-phenylenediamine containing polyimide is partially soluble in dimethyl sulfoxide, tetramethyl urea, N,N-dimethyl acetamide and soluble in methane sulfonic acid and sulfuric acid.
Alvarado, M.↗
Development of Low Density Titanium Alloys for Structural Applications
In this report the results of a program designed to reduce the density of titanium by adding magnesium are presented. Because these two elements are immiscible under conventional ingot metallurgy techniques, two specialized powder metallurgy methods namely, mechanical alloying (MA) and physical vapor deposition (PVD) were implemented. The mechanical alloying experiments were done both at the University of Idaho and at the Defense Research Agency in UK. Since titanium is reactive with interstitial elements, a secondary goal of this research was to correlate solubility extensions with interstitial contamination content, especially oxygen and nitrogen. MA was carried out in SPEX 8000 shaker mils and different milling containers were utilized to control the level of contamination. Results showed that solubilities of Mg in Ti were obtained up to 28 at.% (16.4 wt. %) Mg in Ti for Ti-39.6 at. % (25 wt. %) Mg alloys, which greatly exceed those obtained under equilibrium conditions. This reflects a density reduction of approximately 26 %. Contamination of oxygen and nitrogen seemed to increase the solubility of magnesium in titanium in some cases; however, we were not able to make a clear correlation between contamination levels with solubilities. Work at the DRA has emphasized optimization of present PVD equipment, specifically composition and temperature control. Preliminary PVD data has shown Ti-Mg deposits have successfully been made up to 2 mm thick and that solubility extensions were achieved. The potential for density reduction of titanium by alloying with magnesium has been demonstrated; however, this work has only scratched the surface of the development of such low density alloys. Much research is needed before such alloys could be implemented into industry. Further funding is required in order to optimize the MA/PVD processes including contamination control, determination of optimal alloy compositions, microstructure development, and mechanical property determination.
Froes, F. H.↗