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Highly-alkaline (pH > 12.5) meteoric waters of a Ca 2+ OH − -type issue from naturally calcined bituminous marl. The cold (16.5 ≤ T (°C) ≤ 19.1) waters are super-saturated with minerals thought to be of high-temperature origin.
Uranium and thorium are concentrated in Cretaceous limestone, chert, ash, basalt, and other rock types at Deep Sea Drilling Project Site 465 located on the southern Hess Rise in the central North Pacific. U concentrations, up to 194 ppm on a carbonate-free basis, are among the highest recorded for any deep-sea deposits. U was initially derived from seawater and concentrated by absorption on terrigenous (humic) organic matter in limestone in a shallow marine environment. U and Th were probably concentrated further by low-temperature hydrothermal fluids emanating from the basaltic basement. Mainly montmorillonite, an alteration product of basalt and ash, and organic matter in sedimentary rocks acted as hosts for U and Th. The unique combination of sediments rich in humic organic matter, abundant smectite in altered ash and basalt, and warm hydrothermal solutions provided the necessary conditions for migration and concentration of U and Th. To better understand the conditions limiting the migrating and concentration of U and Th, other rocks deposited during the ocean-wide Cretaceous anoxic events should be analyzed for these elements. ?? 1982.
Core samples of Devonian shales from five localities in the Appalachian basin have been analyzed chemically and mineralogically. The amounts of major elements are similar; however, the minor constituents, organic C, S, phosphate and carbonate show ten-fold variations in amounts. Trace elements Mo, Ni, Cu, V, Co, U, Zn, Hg, As and Mn show variations in amounts that can be related to the minor constituents. All samples contain major amounts of quartz, illite, two types of mixed-layer clays, and chlorite in differing quantities. Pyrite, calcite, feldspar and kaolinite are also present in many samples in minor amounts. Dolomite, apatite, gypsum, barite, biotite and marcasite are present in a few samples in trace amounts. Trace elements listed above are strongly controlled by organic C with the exception of Mn which is associated with carbonate minerals. Amounts of organic C generally range from 3 to 6%, and S is in the range of 2-5%. Amounts of trace elements show the following general ranges in ppm (parts per million): Co, 20-40; Cu, 40-70; U, 10-40; As, 20-40; V, 150-300; Ni, 80-150; high values are as much as twice these values. The organic C was probably the concentrating agent, and the organic C and sulfide S together created an environment that immobilized and preserved these trace elements. Closely spaced samples showing an abrupt transition in color also show changes in organic C, S and trace-element contents. Several associations exist between mineral and chemical content. Pyrite and marcasite are the only minerals found to contain sulfide-S. In general, the illite-chlorite mixed-layer clay mineral shows covariation with organic C if calcite is not present. The enriched trace elements are not related to the clay types, although the clay and organic matter are intimately associated as the bulk fabric of the rock. ?? 1982.
To understand the processes responsible for the presence of low-molecular-weight hydrocarbons (C1-C4) in anoxic environments, we studied sediments collected from an anaerobic estuarine mudflat. In these sediments methane (C1) was several orders of magnitude more abundant than all other C2-C4 hydrocarbons; the C1 (C2 + C3) ratio was ??? 13,000. Mean ethane/ethene and propane/propene ratios were 0.4 and 0.7, respectively. Production of C1-C4 hydrocarbons was monitored during prolonged incubation (7 months) of sediments at 27?? and 4??C. Samples stored at 27??C generated significant quantities of C1-C4 hydrocarbon gases. Incubation at 4??C inhibited production of these gases. Several bactericides were tested with respect to their ability to inhibit formation of gaseous hydrocarbons. Sodium azide, chloroform, and 2-bromoethanesulfonic acid effectively inhibited methane formation, but not ethene formation in dilute continuously-shaken sediment slurries. Zephiran chloride only caused partial inhibition of methanogenesis (46%) and ethene generation (34%) in these slurries. In experiments with more concentrated unshaken sediment slurries, however, zephiran chloride and sodium azide did not block formation of methane, ethane, or propane. Only storage at -10??C prevented production of these gases. These results indicate that C1-C4 hydrocarbons can be formed by low-temperature reactions, possibly mediated by microorganisms. ?? 1982.
Studies of stream and sediment-pore waters largely explain the genesis of concretionary Mn-Fe-oxides in Maine. Waters of two small streams near Jackman, Maine, were studied in terms of pH, Eh, dissolved oxygen, dissolved organic carbon, dissolved Mn, total dissolved Fe, and ferrous and ferric Fe. Pyrite Creek has profuse concretions and coatings of Mn-Fe-oxides, whereas West Pyrite Creek has only sparse Mn-Fe-oxide stains. Pyrite Creek drains boggy terrain and West Pyrite Creek drains well-drained terrain. In West Pyrite Creek, stream and subjacent pore waters have chemical characteristics that do not differ greatly. However, dissolved Mn, ferrous Fe, dissolved oxygen, and in situ Eh measurements show that a steep Eh gradient exists between stream and subjacent pore waters of Pyrite Creek. The steep Eh gradient is manifested by the common zonation of coatings and stains on rocks in stream sediment. The bottom zone has no deposition of oxides, the middle zone is red and consists mostly of Fe-oxides, and the upper zone is black or dark-brown and consists of Mn-oxides with varying amounts of Fe-oxides. The zonation agrees with theoretical predictions of oxide stability as one moves from a reducing to an oxidizing environment. At locations where concretionary Mn-Fe-oxides form, pore waters are depleted of oxygen because of abundant decaying organic material in the stream sediment. The pore waters are charged with dissolved Mn and Fe because mechanically deposited Mn-Fe-oxides are remobilized due to the low-Eh conditions. Groundwaters also contribute dissolved Mn and Fe. Stream waters, on the other hand, are oxygenated and the high-Eh conditions result in low concentrations of dissolved Mn and Fe in stream waters because of the insolubility of Mn-Fe-oxides in high-Eh environments. Therefore, concretionary Mn-Fe-oxides form at the interface between pore and stream waters because Mn- and Fe-rich pore waters, which are undersaturated with respect to Mn-Fe-oxides, mix with oxygen-rich stream waters, which are saturated with respect to Mn-Fe-oxides. ?? 1983.
Two types of basalt (a high-Al basalt associated with the rhyolitic centres north of Taupo and a "low-Al" basalt erupted from Red Crater, Tongariro Volcanic Centre) and five types of andesite (labradorite andesite, labradorite-pyroxene andesite, hornblende andesite, pyroxene low-Si andesite and olivine andesite/low-Si andesite) occur in the Taupo Volcanic Zone (TVZ), North Island, New Zealand. Rare-earth abundances for both basalts and andesites are particularly enriched in light rare-earth elements. High-Al basalts are more enriched than the "low-Al" basalt and have values comparable to the andesites. Labradorite and labradorite-pyroxene andesites all have negative Eu anomalies and hornblende andesites all have negative Ce anomalies. The former is probably due to changing plagioclase composition during fractionation and the latter to late-stage hydration of the magma. Least-squares mixing models indicate that neither high-Al nor "low-Al" basalts are likely sources for labradorite/labradorite-pyroxene andesites. High-Al basalts are considered to result from fractionation of olivine and clinopyroxene from a garnet-free peridotite at the top of the mantle wedge. Labradorite/labradorite-pyroxene andesites are mainly associated with an older NW-trending arc. The source is likely to be garnet-free but it is not certain whether the andesites result from partial melting of the top of the subducting plate or a hydrated lower portion of the mantle wedge. Pyroxene low-Si andesites probably result from cumulation of pyroxene and calcic plagioclase within labradorite-pyroxene andesites, and hornblende andesites by late-stage hydration of labradorite-pyroxene andesite magma. Olivine andesites, low-Si andesites and "low-Al" basalts are related to the NNE-trending Taupo-Hikurangi arc structure. Although the initial source material is different for these lavas they have probably undergone a similar history to the labradorite/labradorite-pyroxene andesites. All lavas show evidence of crustal contamination. ?? 1983.
Eleven analyzed lava samples from Ponape Island are alkali olivine basalt, basanite and basanitoid. Most lavas are aphyric or sparsely phyric (< 10% phenocrysts) and have phenocrysts of olivine (Fo77-80), clinopyroxene and titanomagnetite, and microphenocrysts of plagioclase (An53-68) in a fine-grained groundmass of olivine, clinopyroxene, plagioclase, opaques, potassic oligoclase, ?? nepheline and accessary phases. Oxygen isotope and Fe2O3 FeO data suggest that most samples are fresh, although H2O contents are high. Xenoliths of chromite-bearing harzburgites and dunites, both with cumulate textures occur in one locality. Major- and trace-element concentrations are similar to other oceanic volcanic islands. Most major elements and compatible trace elements vary systematically with respect to the Mg number [ 100Mg (Mg + Fe2+)]. In contrast, the incompatible trace elements do not correlate with the Mg number, but do covary with other incompatible elements. Simple closed-system shallow fractionation cannot be invoked to explain the observed chemical variation in the lavas. Derivation of the fractionated lavas (Mg number = 66-48) probably involved polybaric crystal fractionation from a high-Mg-number parental liquid. In addition, variable-source concentration of a trace-element-rich minor phase is postulated. However, the mantle was homogeneous with respect to the ratio of 87Sr 86Sr. New KAr age data are not consistent with the hypothesis that Ponape and the Caroline Ridge represent a simple "hot spot". ?? 1984.
A pilot study was carried out on two relatively deep drill-cores (∼ 600 m) from the Götemar Granite massif in S.E. Sweden. This granite is typical of the 1400-Ma anorogenic granites of the northern hemisphere. Samples from representative, unfractured parts of the cores, together with four samples taken along a profile tangential to a fracture plane at ∼ 280-m depth, were investigated chemically, mineralogically and isotopically. The results show that after crystallisation, subtle and pervasive open-system modifications of the trace-element chemistry of the granite took place. Whereas the major-element chemistry and minera-logical data emphasised the relative homogeneity of the Götemar Granite samples investigated, trace elements such as U, Rb, and Pb revealed irregular distributions which are probably the result of large-scale hydrothermal alteration processes. This conclusion is supported by isotopic studies which indicate that whole-rock samples were open to a gain or loss of Pb and possibly U at ∼ 420 ± 171 Ma ago. In addition, isotopic data for U-Pb and U-Ra are consistent with a recent minor loss of U. The pervasive alteration and the more recent mobilisation of U are evident to a depth of at least 600 m. The effects are most prevalent along major fracture zones and within the upper 250–300 m of one drill-hole where a high frequency of crush zones has been noted. Higher Fe oxidation ratios, higher Rb contents, lower U contents and correspondingly higher Th/U ratios, all characterise this zone.
Low-temperature (120??C and less) metamorphism of graywacke, granite and andesite yields zeolites and precursor gels by reaction with fresh water but low-greenschist facies by reaction with salt (sea)water. ?? 1985.
Experimental chemical weathering of the so-called Old Rag Granite and Massanutten Sandstone, Virginia, U.S.A., has produced a comparison with the natural environment, and prediction of the effect of acid precipitation. The experimental results of the release of elements, dissolution of minerals, total rock weathered and the degree of weathering as function of volume of leachate were plotted. These data were compared with the natural environment. The use of the plots to predict the effect of high levels of rain acidity on weathering of these rocks is demonstrated. A nonexpandable 14-Å clay was developed from the alteration of biotite during the experimental chemical weathering of the granite at pH 4. This interstratified Al(OH)—mica clay resembles those of the soil developed on the granite and sandstone. Hydroxy-Al may be precipitating between the mica interlayers and producing a 14-Å spacing. Development of this clay by chemical alteration of biotite may change the current hypotheses about its origin in the soils of northeastern U.S.A. While Al-hydroxide seems to regulate Al concentrations in stream waters at the present level of rain acidity, it was found that at lower pH and in the presence of high sulfate concentrations, Al solubility may be controlled by Al-sulfate phase(s).
D/H and 18O 16O ratios have been determined for fumarole condensates from Augustine Volcano, an active calc-alkaline stratovolcano in Lower Cook Inlet, Alaska. The isotopic data for the condensates form a linear ?? D-?? 18O array from low-temperature fluids (< 100??C) which are essentially local meteoric water (?? D {reversed tilde equals} -150???, ?? 18O {reversed tilde equals} -19???) to high-temperature (>450??C) fluids collected at the volcano summit which are enriched in both D and 18O (?? D {reversed tilde equals} -35???, ?? 18O {reversed tilde equals} +3.5???). Several lines of evidence suggest that the D-and 18O-rich condensates likely are "magmatic" fluids released into the hydrothermal system during and immediately after the 1976 eruption. Prior to 1976, the Augustine hydrothermal system was dominated completely by local meteoric waters. Between 1976 and 1982, fumarole condensates were observed to be variable mixtures of the "magmatic" fluid and meteoric water, with the proportion of the former systematically decreasing as the hydrothermal system cooled following the 1976 eruption. ?? 1985.
Measurements were made of the hydrogen isotope composition of 74 samples of muscovite, biotite, vein quartz and whole rocks from the Papoose Flat pluton, eastern California, U.S.A., and adjacent metamorphic and sedimentary rocks in order to elucidate the genesis and evolution of water and hydrous minerals in a two-mica granodiorite. Electron microprobe analyses were made of all micas so that the Suzuoki-Epstein equation could be used in evaluating the data. Based on experimental, theoretical and textural evidence of mica paragenesis, a model of hydrogen isotope fractionation between an aqueous vapor and a magma during crystallization has been constructed. This model accounts for the observed hydrogen isotope relations and implies that primary hydrogen isotope compositions have been preserved in a large portion of the pluton. The ?? D-values of biotites vary widely over the range -103 to -66% with most values lying between -90 and -70??? Muscovites, on the other hand, are isotopically more uniform and have ?? D-values of -61 to -41??? with most values lying between -50 and -46??? These data are consistent with the interpretation that biotite formed over a long period of crystallization whereas muscovite formed in a narrow interval, presumably during the final stages of crystallization when alumina and water contents were at their highest. Only 8 of the 21 muscovite-biotite pairs analyzed are in hydrogen isotope equilibrium as calculated from the Suzuoki-Epstein equation. Biotites in the western half of the pluton have relatively low ?? D-values of around -85???, whereas those in the eastern half have higher values of up to -66??? This pattern is a consequence of a loss of permeability associated with the syn-intrusive deformation of the western margin of the pluton. This loss of permeability enhanced the preservation of primary hydrogen isotope relations there by diverting water evolved from the magma out through the eastern half of the pluton where some deuteric exchange is documented. A much larger metamorphic aureole with extensive retrograde textures around the eastern end of the pluton attests to the passage of this water. ?? 1985.
Six analytical techniques for the selective chemical dissolution of sulfides are compared with the purpose of defining the best method for accurately determining the concentration of sulfide-bound nickel. Synthesized sulfide phases of known elemental content, mixed with well-analyzed silicates, were used to determine the relative and absolute efficiency, based on Ni and Mg recovery, of the techniques. Tested leach-methods purported to dissolve sulfide from silicate phases include: brominated water, brominated water-carbon tetrachloride, nitric-hydrochloric acid, hydrogen peroxide-ammonium citrate, bromine-methanol and hydrogen peroxide-ascorbic acid. Only the hydrogen peroxide-ammonium citrate method did not prove adequate in dissolving the sulfide phases. The remaining five methods dissolved the sulfide phases, but the indicated amount of attack on the silicate portion ranged from 3% to 100%. The bromine-methanol method is recommended for assaying sulfide-Ni deposits when Ni is also present in silicate phases. ?? 1986.
Several methods have been developed and used to extract and chemically analyze the two major types of fluid inclusions in bedded salt from the Palo Duro Basin, Texas. Data on the ratio K: Ca: Mg were obtained on a few of the clouds of tiny inclusions in "chevron" salt, representing the brines from which the salt originally crystallized. Much more complete quantitative data (Na, K, Ca, Mg, Sr, Cl, SO4 and Br) were obtained on ??? 120 individual "large" (mostly ???500 ??m on an edge, i.e., ??? ??? 1.6 ?? 10-4 g) inclusions in recrystallized salt. These latter fluids have a wide range of compositions, even in a given piece of core, indicating that fluids of grossly different composition were present in these salt beds during the several (?) stages of recrystallization. The analytical results indicating very large inter-and intra-sample chemical variation verify the conclusion reached earlier, from petrography and microthermometry, that the inclusion fluids in salt and their solutes are generally polygenetic. The diversity in composition stems from the combination of a variety of sources for the fluids (Permian sea, meteoric, and groundwater, as well as later migrating ground-, formation, or meteoric waters of unknown age), and a variety of subsequent geochemical processes of dissolution, precipitation and rock-water interaction. The compositional data are frequently ambiguous but do provide constraints and may eventually yield a coherent history of the events that produced these beds. Such an understanding of the past history of the evaporite sequence of the Palo Duro Basin should help in predicting the future role of the fluids in the salt if a nuclear waste repository is sited there. ?? 1987.
The chemistry of three stream, three spring and six near-surface waters in the vicinity of a Holocene organic-rich uranium deposit is described, with particular emphasis on the chemistry of U. Results characterize the solution behavior of uranium as U-bearing water interacts with relatively undecomposed, surficial organic matter. Of the measured major and trace chemical species, only U is consistently highly enriched (17-318 ppb) relative to reported values for regional waters, or to literature values for waters in largely granitic terrains. R-mode factor analysis of the chemical data suggests that most U is present in a soluble form, but that some U is also associated with fine suspended particulates of clay, organic matter, or hydrous oxides. Calculations that apply thermodynamic data to predict U speciation in solution indicate the relative importance of uranyl carbonate and uranyl phosphate complexes. Analysis of more finely filtered samples (0.05 ??m vs. 0.45 ??m), and direct radiographic observations using fission-track detectors suspended in the waters indicate the presence of some uraniferous particulate matter. Application of existing thermodynamic data for uranous- and uranyl-bearing minerals indicates that all waters are undersaturated with U minerals as long as ambient Eh ??? +0.1 v. If coexisting surface and near-surface waters are sufficiently oxidizing, initial fixation of U in the deposit should be by a mechanism of adsorption. Alternatively, more reducing conditions may prevail in deeper pore waters of the organic-rich host sediments, perhaps leading to direct precipitation or diagenetic formation of U4+ minerals. A 234U 238U alpha activity ratio of 1.08 ?? 0.02 in a spring issuing from a hillslope above the deposit suggests a relatively soluble source of U. In contrast, higher activity ratios of 234U 238U (??? 1.3) in waters in contact with the uraniferous valley-fill sediments suggest differences in the nature of interaction between groundwater and the local, U-rich source rocks. ?? 1987.
Six cores, ranging in length from 1 to 2 m, were collected in the Cheyenne River arm of Lake Oahe, South Dakota, to investigate potential impacts from gold-mining operations around Lead, South Dakota. Sedimentation rates in the river arm appear to be event-dominated and rapid, on the order of 6-7 cm yr.-1. All the chemical concentrations in the core samples fall within the wide ranges previously reported for the Pierre Shale of Cretaceous age and with the exception of As, generally are similar to bed sediment levels in the Cheyenne River, Lake Oahe and Foster Bay. Based on the downcore distribution of Mn, it appears that reducing conditions exist in the sediment column of the river arm below 2-3 cm. The reducing conditions do not appear to be severe enough to produce differentiation of Fe and Mn throughout the sediment column in the river arm. Cross-correlations for high-level metal-bearing strata within the sediment column can be made for several strata and for several cores; however, cross-correlations for all the high-level metal-bearing strata are not feasible. As is the only element which appears enriched in the core samples compared to surface sediment levels. Well-crystallized arsenopyrite was found in high-As bearing strata from two cores and probably was transported in that form from reducing sediment-storage sites in the banks or floodplains of Whitewood Creek and the Belle Fourche River. It has not oxidized due to the reducing conditions in the sediment column of the Cheyenne River arm. Some As may also be transported in association with Fe- and Mn-oxides and -hydroxides, remobilized under the reducing conditions in the river arm, and then reprecipitated in authigenic sulfide phases. In either case, the As appears to be relatively immobile in the sediment column. ?? 1988.
The clay-hill nitrate deposits of the Amargosa River valley, California, are caliche-type accumulations of water-soluble saline minerals in clay-rich soils on saline lake beds of Miocene, Pliocene(?) and Pleistocene age. The soils have a maximum thickness of ??? 50 cm, and commonly consist of three layers: (1) an upper 5-10 cm of saline-free soil; (2) an underlying 15-20 cm of rubbly saline soil; and (3) a hard nitrate-rich caliche, 10-20 cm thick, at the bottom of the soil profile. The saline constituents, which make up as much as 50% of the caliche, are chiefly Cl-, NO-3, SO2-4 and Na+. In addition are minor amounts of K+, Mg2+ and Ca2+, varying, though generally minor, amounts of B2O3 and CO2-3, and trace amounts of I (probably as IO-3), NO-2, CrO2-4 and Mo (probably as MoO2-4). The water-soluble saline materials have an I/Br ratio of ??? 1, which is much higher than nearly all other saline depostis. The principal saline minerals of the caliche are halite (NaCl), nitratite (NaNO3), darapskite (Na3(SO4)(NO3)??H2O), glauberite (Na2Ca(SO4)2), gypsum (CaSO4??2H2O) and anhydrite (CaSO4). Borax (Na2B4O5(OH)4??8H2O), tincalconite (Na2B4O5(OH)4??3H2O) and trona (Na3(CO3)(HCO3)??2H2O) are abundant locally. The clay-hill nitrate deposits are analogous to the well-known Chilean nitrate deposits, and probably are of similar origin. Whereas the Chilean deposits are in permeable soils of the nearly rainless Atacama Desert, the clay-hill deposits are in relatively impervious clay-rich soils that inhibited leaching by rain water. The annual rainfall in the Death Valley region of ??? 5 cm is sufficient to leach water-soluble minerals from the more permeable soils. The clay-hill deposits contain saline materials from the lake beds beneath the nitrate deposits are well as wind-transported materials from nearby clay-hill soils, playas and salt marshes. The nitrate is probably of organic origin, consisting of atmospheric nitrogen fixed as protein by photoautotrophic blue-green algae, which are thought to form crusts on soils at the sites of the deposits when moistened by rainfall. The protein is subsequently transformed to nitrate by autotophic bacteria. ?? 1988.
Three distinct types of solid material are associated with each sample of the hydrothermal fluid that was collected from the vents of the Southern Juan de Fuca Ridge. The solid materials appear to be representative of deposits on ocean floors near mid-ocean ridges, and interpretation of the chemistry of the hydrothermal solutions requires understanding of them. Sr isotopic evidence indicates that at least two and probably all three of these solid materials were removed from the solution with which they are associated, by precipitation or adsorption. This occurred after the "pure" hydrothermal fluid was diluted and thoroughly mixed with ambient seawater. The three types of solid materials, are, respectively, a coarse Zn- and Fe-rich material with small amounts of Na and Ca; a finer material also rich in Zn and Fe, but with alkali and alkaline-earth metals; and a scum composed of Ba or Zn, with either considerable Fe or Si, and Sr. Mineral identification is uncertain because of uncertain anion composition. Only in the cases of Ba and Zn were metal masses greater in solid materials than in the associated fluids. For all other metals measured, masses in fluids dwarf those in solids. The fluids themselves contain greater concentrations of all metals measured, except Mg, than seawater. We discuss in detail the relative merits of two methods of determining the mixing proportions of "pure" hydrothermal solution and seawater in the fluids, one based on Sr isotopes, and another previously used method based on Mg concentrations. Comparison of solute concentrations in the several samples shows that degree of dilution of "pure" hydrothermal solutions by seawater, and amounts of original solutes that were removed from it as solid materials, are not related. There is no clear evidence that appreciable amounts of solid materials were not conserved (lost) either during or prior to sample collection. ?? 1988.