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1.
The high field strength elements (HFSE: Zr, Hf, Nb, Ta, and W) are an important group of chemical tracers that are increasingly used to investigate magmatic differentiation processes. Successful modeling of these processes requires the availability of accurate mineral-melt partition coefficients (D). To date, these have largely been determined by ion microprobe or laser ablation-ICP-MS analyses of the run products of high-pressure, high-temperature experiments. Since HFSE are (highly) incompatible, relatively immobile, high-charge, and difficult to ionize, these experiments and their analysis are challenging. Here we explore whether high-precision analyses of natural mineral-melt systems can provide additional constraints on HFSE partitioning.The HFSE concentrations in natural garnet and amphibole and their alkaline host melt from Kakanui, New Zealand are determined with high precision isotope dilution on a multi-collector-ICP-MS. Major and trace element compositions combined with Lu-Hf isotopic systematics and detailed petrographic sample analysis are used to assess mineral-melt equilibrium and to provide context for the HFSE D measurements. The whole-rock nephelinite, ∼1 mm sized amphiboles in the nephelinite, and garnet megacrysts have similar initial Hf isotope ratios with a mean initial 176Hf/177Hf(34 Ma) = 0.282900 ± 0.000026 (2σ). In contrast, the amphibole megacrysts are isotopically distinct (176Hf/177Hf(34 Ma) = 0.282830 ± 0.000011). Rare earth element D values for garnet megacryst-nephelinite melt and ∼1 mm amphibole-nephelinite melt plotted as a function of ionic radii show classic near-parabolic trends that are in excellent agreement with crystal lattice-strain models. These observations are consistent with equilibrium between the whole-rock nephelinite, the ∼1 mm amphibole grains within the nephelinite and the garnet megacrysts.High-precision isotope dilution results for Zr and Hf in garnet (DZr = 0.220 ± 0.007 and DHf = 0.216 ± 0.005 [2σ]), and for all HFSE in amphibole are consistent with previous experimental findings. However, our measurements for Nb and Ta in garnet (DNb = 0.0007 ± 0.0001 and DTa = 0.0011 ± 0.0006 [2σ]) show that conventional methods may overestimate Nb and Ta concentrations, thereby overestimating both Nb and Ta absolute D values for garnet by up to 3 orders of magnitude and underestimating DNb/DTa by greater than a factor of 100. As a consequence, the role of residual garnet in imposing Nb/Ta fractionation may be less important than previously thought. Moreover, garnet DHf/DW = 17 and DNb/DZr = 0.003 imply fractionation of Hf from W and Nb from Zr upon garnet crystallization, which may have influenced short-lived 182Hf-182W and 92Nb-92Zr isotopic systems in Hadean time.  相似文献   

2.
The partitioning of a number of trace elements (Ba, Nb, Zr, Y, REE, etc.) between orthopyroxene, garnet, and carbonate-silicate melt was experimentally studied using a belt apparatus at pressures of 3.5–4.2 GPa and temperatures of 1300–1500°C. The experimental products were investigated by electron microprobe analysis and laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). The experimental melts varied from carbonatitic (～5 wt % SiO2) at low temperatures (1300–1350°C) to kimberlitic compositions (30 wt % SiO2) at high temperatures (1500°C). The partition coefficients of most elements between orthopyroxene and melt (D i Opx/L ) and garnet and melt (D i Grt/L ) were almost independent of melt composition (temperature). The D i Opx/L values ranged from <0.01 for the most incompatible Ba and light REE to 0.02–0.08 for moderately incompatible Zr, Y, and heavy REE. The D i Grt/L values were approximately an order of magnitude higher, ～0.07 for light REE, 0.7 for Y, and 1.5 for Yb. The character of D i Grt/L variations in the systems studied is in general similar to that established for silicate melts without volatile components. However, the differences in the behavior of moderately incompatible and compatible elements (e.g., light and heavy REE) in the experimental systems are less pronounced compared with CO2-free systems. Considering carbonate-silicate and silicate melts as possible agents of mantle metasomatism, it can be concluded that the former can efficiently transport heavy REE, and the latter have a greater affinity for Nb, Ba, and light REE. A characteristic feature of mantle rocks enriched by carbonate-silicate melts is high Ba/La ratio coupled with relatively weakly fractionated REE distribution patterns. It was shown that the high degrees of enrichment observed in natural kimberlites can be explained by a two-stage scenario, including a preliminary invasion of carbonate-silicate melt into depleted harzburgites in the lower parts of the lithosphere and subsequent very low degree melting.  相似文献   

3.
Highly anhydrous granulites from Río Santa Rosa in the eastern Sierras Pampeanas of Argentina occur as a thick lens surrounded by melt-depleted migmatites. Grt–Crd granulite composed of Qtz+Pl+Grt+Crd+Ilm±Spl±Ath±Phl is the dominant rock, whereas Opx–Grt granulite appears as discontinuous lenses in the center of the granulite body. Grt–Crd granulite includes blocks of metabasite that are relics of refractory lithologic beds interlayered in the supracrustal sequence. A distinct assemblage composed of Qtz, Pl, Grt, Crd, Opx, Spl, Crn, Sil, Bt, Phl, Ath, and Fe–Ti oxides in different combinations was generated in a reaction zone between Grt–Crd granulites and metabasites at peak metamorphism (850–900 °C and 7.6±0.5 kbar). The P–T trajectory of Grt–Crd granulites suggests an early prograde garnet-forming stage followed by nearly isothermal decompression that caused garnet breakdown. Melting and melt draining accompanying garnet growth was active during heating (to 900 °C) at intermediate pressures (∼7.6 kbar). Peak P–T estimates for Opx–Grt granulites are similar to those obtained with Grt–Crd granulites, which indicates that both granulites passed through the highest thermal stage. These results constrain the late evolution of Opx–Grt granulite to a garnet-consuming stage. Furthermore, they imply that garnet formation in Opx–Grt granulite happened at an early prograde P–T trajectory. Garnet growth in Opx–Grt granulite cannot result from heating at high pressure, which would lead to an apparent contradiction in the prograde P–T paths of the two granulites. This discrepancy may be solved by demonstrating that Opx–Grt granulite is the product of synmetamorphic mafic magmatism that was contaminated while cooling. The Río Santa Rosa granulites are inferred to have formed in a thickened crust in which mafic magmatic activity providing a local heat input.  相似文献   

4.
The prograde deserpentinized peridotites from the talc zone in the Happo-O’ne complex, central Japan, show differences in their field relation and mineral assemblage with the high-P retrograde peridotites of the other part of the complex. They show a mineral assemblage, olivine + talc + antigorite ± prograde tremolite ± chlorite, formed by thermal metamorphism around the granitic intrusion at T, 500-650 °C and P < 7 kbar. The olivine has numerous opaque inclusions and high Fo (91.5-96.5) relative to the retrograde olivine, reflecting its formation by deserpentinization. The prograde tremolite, which is low in Al2O3 (<1.0 wt.%), Cr2O3 (<0.35 wt.%), and Na2O (<0.6 wt.%) but high in Mg# (up to 0.98) and SiO2 (up to 59.9 wt.%), is different in size, shape and chemistry from the retrograde tremolite. The prograde peridotites display a U-shaped REE pattern (0.02-0.5 times PM), similar to diopside-zone retrograde metaperidotites, possible protoliths. They are enriched in LILE (e.g., Cs, Pb, Sr, Rb) relative to HFSE (e.g., Ta, Hf, Zr, Nb), like their protoliths, because of their local re-equilibration with the fluid released during dehydration of the protoliths. They have high contents of REE and some trace elements (e.g., Cs, Th, U, Ta) relative to their protoliths because of an external-element addition from the granitic magma. In-situ analyses of peridotitic silicates confirmed that the prograde tremolite and talc display a spoon-shaped primitive mantle (PM)-normalized REE pattern (0.1-3 times PM) in which LREE are higher than HREE contents. The prograde tremolite is depleted in Al, Na, Cr, Sc, V, Ti, B, HREE and Li, but is enriched in Si, Cs, U, Th, HFSE (Hf, Zr, Nb, Ta), Rb and Ba relative to the retrograde tremolite; the immobile-element depletion in this tremolite is inherited from its source (antigorite + secondary diopside), whereas the depletion of mobile elements (e.g., Li, B, Na, Al) is ascribed to their mobility during the deserpentinization and/or the depleted character of the source of tremolite. The enrichment of HFSE and LILE in the prograde tremolite is related to an external addition of these elements from fluid/melt of the surrounding granitic magma and/or in situ equilibrium with LILE-bearing fluid released during dehydration of serpentinized retrograde metaperidotites and olivine-bearing serpentinites (protoliths). The prograde olivine is higher in REE and most trace-element contents than the retrograde one due to the external addition of these elements; it is enriched in B, Co and Ni, but depleted in Li that was liberated during deserpentinization by prograde metamorphism.  相似文献   

5.
The hafnium isotope composition of Pacific Ocean water   总被引：1，自引：0，他引：1  
The first Hf isotope data for seawater are reported for a series of stations in the Northwestern Pacific and define a range from εHf = 3.5 ± 1.4 to 8.6 ± 1.6. Most samples have values within error of the average of εHf = 5.9, but significant variations are found in intermediate waters at a depth of 600 m, as well as in deep waters. The Nd and Hf isotope compositions of the deep waters fall within the range of values found for surfaces of hydrogenetic ferromanganese crusts in the region, confirming that Hf in the Fe-Mn crusts has been derived from the overlying water column, which thus provide an archive of past seawater compositions. Although the seawater samples are generally close to the global εNd-εHf correlation obtained from ferromanganese crusts, there are significant deviations from this correlation indicating that there is some additional decoupling between Nd and Hf isotope signals, most likely caused by local water mass mixing and differences in residence times. This is not resolved in the crust samples, which integrate seawater signals over 104 years. The combined use of these two isotope systems in seawater therefore provides an additional dimension for tracing water masses in the oceans. Studies of the distribution of oceanic Hf isotope compositions that have been confined to deep water and boundary waters, as recorded in seafloor ferromanganese crusts, can now be extended and aimed at characterising the entire present-day water column. Average Hf concentrations measured in this study are somewhat lower than previously reported, suggesting a shorter residence time for Hf in the global oceans, although the uncertainty in the extent of Hf removal from the water column during estuarine mixing as well as a lack of data on hydrothermal and dust inputs remains a limit on how well the residence time can be defined.  相似文献   

6.
We have carried out a Pb double-spike and Lu-Hf isotope study of clinopyroxenes from spinel-facies mantle xenoliths entrained in Cenozoic intraplate continental volcanism of the French Massif Central (FMC). U-Th-Pb and Lu-Hf isotope systematics verify the existence of different lithospheric domains beneath the northern and southern FMC. Northern FMC clinopyroxenes have extreme Lu/Hf ratios and ultra-radiogenic Hf (εHf = +39.6 to +2586) that reflect ∼15-25% partial melting in Variscan times (depleted mantle model ages ∼360 Ma). Zr, Hf and Th abundances in these clinopyroxenes are low and unaffected by hydrous/carbonatitic metasomatism that overprinted LILE and light REE abundances and caused decoupling of Lu/Hf-Sm/Nd ratios and Nd-Hf isotopes (εNd = +2.1 to +91.2). Pb isotopes of northern FMC clinopyroxenes are radiogenic (206Pb/204Pb > 19), and typically more so than the host intraplate volcanic rocks. 238U/204Pb ratios range from 17 to 68, and most samples have distinctively low 232Th/238U (<1) and 232Th/204Pb (3-22). Clinopyroxenes from southern FMC lherzolites are generally marked by overall incompatible trace element enrichment including Zr, Hf and Th abundances, and have Pb isotopes that are similar to or less radiogenic than the host volcanic rocks. Hf isotope ratios are less radiogenic (εHf = +5.4 to +41.5) than northern FMC mantle and have been overprinted by silicate-melt-dominated metasomatism that affected this part of FMC mantle. Major element and Lu concentrations of clinopyroxenes from southern FMC harzburgites are broadly similar to northern FMC clinopyroxenes and suggest they experienced similar degrees of melt extraction as northern FMC mantle. 238U/204Pb (53-111) and 232Th/204Pb ratios (157-355) of enriched clinopyroxenes from the southern FMC are extreme and significantly higher than the intraplate volcanic rocks. In summary, mantle peridotites from different parts of the FMC record depletion at ∼360 Ma during Variscan subduction, followed by differing styles of enrichment. Northern FMC mantle was overprinted by a fluid/carbonatitic metasomatic agent that carried elements like U, Pb, Sr and light REE. In contrast, much of the southern FMC mantle was metasomatised by a small-degree partial silicate melt resulting in enrichment of all incompatible trace elements. The extreme mantle 238U/204Pb (northern and southern FMC), 232Th/238U (northern FMC) and 232Th/204Pb ratios (southern FMC), coupled with unremarkable present-day Pb isotope ratios, constrain the timing of enrichment. Mantle metasomatism is a young feature related to melting of the upwelling mantle responsible for Cenozoic FMC volcanism, rather than subduction-related metasomatism intimately associated with mantle depletion during the Variscan orogeny. The varying metasomatic styles relate to pre-existing variations in the thickness of the continental lithospheric lid, which controlled the extent to which upwelling mantle could ascend and melt. In the northern FMC, a thicker and more refractory lithospheric lid (?80 km) only allowed incipient degrees of melting resulting in fluid/carbonatitic metasomatism of the overlying sub-continental lithospheric mantle. The thinner lithospheric lid of the southern FMC (?70 km) allowed larger degrees of melting and resulted in silicate-melt-dominated metasomatism, and also focused the location of the volcanic fields of the FMC above this region.  相似文献   

7.
Hafnium isotopes in Arctic Ocean water   总被引：1，自引：0，他引：1  
The first isotopic compositions of dissolved hafnium in seawater from across the Arctic Ocean are reported. Most samples from the four sub-basins of the Arctic Ocean have values within error of an average of εHf = +0.8. Combined Hf-Nd isotope compositions do not fall on the well-established positive correlation for mantle and crustal rocks. Instead, Arctic waters have Hf that is more radiogenic than that typically found in rocks with similar Nd isotope compositions, a feature previously found in ferromanganese crusts and waters from the Pacific Ocean. Arctic seawater samples generally fall on the lower part of the ferromanganese crust array, reflecting influences of inputs from Arctic rivers and interactions of shelf waters with underlying sediments. Arctic rivers have much higher Hf concentrations (7-30 pM) than Arctic seawater (0.36-4.2 pM). Water from the Mackenzie River has the least radiogenic Hf, with εHf = −7.1 ± 1.7, and plots furthest away from the ferromanganese crust array, while waters from the Ob, Yenisey, and Lena Rivers have values that are indistinguishable from most Arctic waters. In the Amundsen, Makarov, and Canada basins, Hf concentrations are highest at the surface and lowest in the deeper waters, reflecting the influences of riverine inputs and of waters that have flowed over the extensive Siberian continental shelves and have Nd and Hf characteristics that reflect water-sediment interactions. This is in contrast to the relatively low near surface Hf concentrations reported for locations elsewhere. The Pacific water layer in the Canada Basin exhibits the highest value of εHf = +6.8 ± 1.8, reflecting the Hf isotopic composition of waters entering the Arctic from the Pacific Ocean. Mixing relationships indicate that a substantial fraction of the Hf in the Mackenzie River is lost during estuarine mixing; the behaviour of Hf from other rivers is less constrained.  相似文献   

8.
This paper presents new major and trace-element data and Lu-Hf and Sm-Nd isotopic compositions for representative suites of marine sediment samples from 14 drill sites outboard of the world’s major subduction zones. These suites and samples were chosen to represent the global range in lithology, Lu/Hf ratios, and sediment flux in subducting sediments worldwide. The data reported here represent the most comprehensive data set on subducting sediments and define the Hf-Nd isotopic variations that occur in oceanic sediments and constrain the processes that caused them.Using new marine sediment data presented here, in conjunction with published data, we derive a new Terrestrial Array given by the equation, εHf = 1.55 × εNd + 1.21. This array was calculated using >3400 present-day Hf and Nd isotope values. The steeper slope and smaller y-intercept of this array, compared to the original expression (εHf = 1.36 × εNd + 2.89; Vervoort et al., 1999) reflects the use of present day values and the unradiogenic Hf of old continental samples included in the array.In order to examine the Hf-Nd isotopic variations in marine sediments, we have classified our samples into 5 groups based on lithology and major and trace-element geochemical compositions: turbidites, terrigenous clays, and volcaniclastic, hydrothermal and hydrogenetic sediments. Compositions along the Terrestrial Array are largely controlled by terrigenous material derived from the continents and delivered to the ocean basins via turbidites, volcaniclastic sediments, and volcanic inputs from magmatic arcs. Compositions below the Terrestrial Array derive from unradiogenic Hf in zircon-rich turbidites. The anomalous compositions above the Terrestrial Array largely reflect the decoupled behavior of Hf and Nd during continental weathering and delivery to the ocean. Both terrigenous and hydrogenetic clays possess anomalously radiogenic Hf, reflecting terrestrial sedimentary and weathering processes on the one hand and marine inheritance on the other. This probably occurs during complementary processes involving preferential retention of unradiogenic Hf on the continents in the form of zircon and release of radiogenic Hf from the breakdown of easily weathered, high Lu-Hf phases such as apatite.  相似文献   

9.
Although orthopyroxene (Opx) is present during a wide range of magmatic differentiation processes in the terrestrial and lunar mantle, its effect on melt trace element contents is not well quantified. We present results of a combined experimental and computational study of trace element partitioning between Opx and anhydrous silicate melts. Experiments were performed in air at atmospheric pressure and temperatures ranging from 1,326 to 1,420°C in the system CaO–MgO–Al2O3–SiO2 and subsystem CaO–MgO–SiO2. We provide experimental partition coefficients for a wide range of trace elements (large ion lithophile: Li, Be, B, K, Rb, Sr, Cs, Ba, Th, U; rare earth elements, REE: La, Ce, Nd, Sm, Y, Yb, Lu; high field strength: Zr, Nb, Hf, Ta, Ti; transition metals: Sc, V, Cr, Co) for use in petrogenetic modelling. REE partition coefficients increase from $ D_{\text{La}}^{{\text{Opx}} {\hbox{-}} {\text{melt}}} \sim 0.0005 Although orthopyroxene (Opx) is present during a wide range of magmatic differentiation processes in the terrestrial and lunar mantle, its effect on melt trace element contents is not well quantified. We present results of a combined experimental and computational study of trace element partitioning between Opx and anhydrous silicate melts. Experiments were performed in air at atmospheric pressure and temperatures ranging from 1,326 to 1,420°C in the system CaO–MgO–Al2O3–SiO2 and subsystem CaO–MgO–SiO2. We provide experimental partition coefficients for a wide range of trace elements (large ion lithophile: Li, Be, B, K, Rb, Sr, Cs, Ba, Th, U; rare earth elements, REE: La, Ce, Nd, Sm, Y, Yb, Lu; high field strength: Zr, Nb, Hf, Ta, Ti; transition metals: Sc, V, Cr, Co) for use in petrogenetic modelling. REE partition coefficients increase from $ D_{\text{La}}^{{\text{Opx}} {\hbox{-}} {\text{melt}}} \sim 0.0005 $ D_{\text{La}}^{{\text{Opx}} {\hbox{-}} {\text{melt}}} \sim 0.0005 to $ D_{\text{Lu}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.109 $ D_{\text{Lu}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.109 , D values for highly charged elements vary from $ D_{\text{Th}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.0026 $ D_{\text{Th}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.0026 through $ D_{\text{Nb}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.0033 $ D_{\text{Nb}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.0033 and $ D_{\text{U}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.0066 $ D_{\text{U}}^{{{\text{Opx}} {\hbox{-}} {\text{melt}}}} \sim 0.0066 to $ D_{\text{Ti}}^{{\text{Opx}} {\hbox{-}} {\text{melt}}} \sim 0.058 $ D_{\text{Ti}}^{{\text{Opx}} {\hbox{-}} {\text{melt}}} \sim 0.058 , and are all virtually independent of temperature. Cr and Co are the only compatible trace elements at the studied conditions. To elucidate charge-balancing mechanisms for incorporation of REE into Opx and to assess the possible influence of Fe on Opx-melt partitioning, we compare our experimental results with computer simulations. In these simulations, we examine major and minor trace element incorporation into the end-members enstatite (Mg2Si2O6) and ferrosilite (Fe2Si2O6). Calculated solution energies show that R2+ cations are more soluble in Opx than R3+ cations of similar size, consistent with experimental partitioning data. In addition, simulations show charge balancing of R3+ cations by coupled substitution with Li+ on the M1 site that is energetically favoured over coupled substitution involving Al–Si exchange on the tetrahedrally coordinated site. We derived best-fit values for ideal ionic radii r 0, maximum partition coefficients D 0, and apparent Young’s moduli E for substitutions onto the Opx M1 and M2 sites. Experimental r 0 values for R3+ substitutions are 0.66–0.67 ? for M1 and 0.82–0.87 ? for M2. Simulations for enstatite result in r 0 = 0.71–0.73 ? for M1 and ~0.79–0.87 ? for M2. Ferrosilite r 0 values are systematically larger by ~0.05 ? for both M1 and M2. The latter is opposite to experimental literature data, which appear to show a slight decrease in $ r_{0}^{{{\text{M}}2}} $ r_{0}^{{{\text{M}}2}} in the presence of Fe. Additional systematic studies in Fe-bearing systems are required to resolve this inconsistency and to develop predictive Opx-melt partitioning models for use in terrestrial and lunar magmatic differentiation models.  相似文献   

10.
Boninites as windows into trace element mobility in subduction zones   总被引：3，自引：0，他引：3  
Boninites are subduction-related rocks originating from re-melting of highly depleted mantle sources left after extraction of tholeiitic melts. Due to their depleted nature, the incompatible trace element inventory of boninites is virtually entirely inherited from slab components without a significant contribution from the refractory mantle wedge. Thus, boninites constitute an excellent window into processes controlling trace element mobilization at the slab-mantle wedge interface. In order to constrain the behaviour of trace elements in subduction zones with a special emphasis on high field strength elements, we analyzed low-Ca boninites and associated tholeiitic basalts from Cape Vogel, Papua New Guinea (PNG) and compare them with compositions of high-Ca boninites and associated tholeiitic basalts from Cyprus. High-precision HFSE (Nb, Ta, Zr, Hf, W) concentration data of the boninites and associated tholeiitic basalts were obtained by isotope dilution. Major, trace element, and Sr-Nd-Hf-Pb isotope compositions clearly document a significant contribution of slab-derived melts involved in the petrogenesis of the PNG boninites, whereas only fluid-like subduction components were involved in the petrogenesis of the PNG basalts and the Cyprus suite. Low-Ca boninites from PNG are derived from a more refractory mantle source (∼21% depletion) than the high-Ca boninites from Cyprus (∼11% depletion) and their respective tholeiitic precursors (<10% depletion). In agreement with the more depleted nature of their mantle source, boninites exhibit a significantly stronger overprint by slab components. High-precision HFSE data indicate that, in comparison to LILE, a somewhat lower but measurable mobilization of all investigated HFSE in both slab-derived fluids and melts is evident. Modelling calculations demonstrate that the subduction components dominate the LILE budget and also largely control LREE and HFSE abundances in the boninite sources. Notably, the increasing influence of slab-derived fluids results in a decrease of the negative Nb-Ta anomaly, most likely reflecting a similar mobility of Nb-Ta and LREE at higher pressures near the critical point of fluid-melt miscibility. Ratios of Zr/Hf and Nb/Ta in the melt-like slab components dominating in the sources of the PNG boninites were probably fractionated in equilibrium with garnet-amphibolitic mafic oceanic crust. HFSE ratios in the Cyprus boninites are best explained by dehydration of subducted pelagic sediments in the absence of Ti-rich phases such as rutile. Our results also confirm previous assertions that the mobility of HFSE decreases in the order Sb > W-Mo > Nb-Ta > Zr-Hf. Furthermore, Mo-W systematics may provide a potential novel tracer for the amount, composition and redox state of subducted pelagic sediments that contribute to the geochemical budget of intra-oceanic arc systems.  相似文献   

11.
The sodium solubility in silicate melts in the CaO-MgO-SiO2 (CMS) system at 1400 °C has been measured by using a closed thermochemical reactor designed to control alkali metal activity. In this reactor, Na(g) evaporation from a Na2O-xSiO2 melt imposes an alkali metal vapor pressure in equilibrium with the molten silicate samples. Because of equilibrium conditions in the reactor, the activity of sodium-metal oxide in the molten samples is the same as that of the source, i.e., aNa2O(sample) = aNa2O(source). This design also allows to determine the sodium oxide activity coefficient in the samples. Thirty-three different CMS compositions were studied. The results show that the amount of sodium entering from the gas phase (i.e., Na2O solubility) is strongly sensitive to silica content of the melt and, to a lesser extent, the relative amounts of CaO and MgO. Despite the large range of tested melt compositions (0 < CaO and MgO < 40; 40 < SiO2 < 100; in wt%), we found that Na2O solubility is conveniently modeled as a linear function of the optical basicity (Λ) calculated on a Na-free basis melt composition. In our experiments, γNa2O(sample) ranges from 7 × 10−7 to 5 × 10−6, indicating a strongly non-ideal behavior of Na2O solubility in the studied CMS melts (γNa2O(sample) ? 1). In addition to showing the effect of sodium on phase relationships in the CMS system, this Na2O solubility study brings valuable new constraints on how melt structure controls the solubility of Na in the CMS silicate melts. Our results suggest that Na2O addition causes depolymerization of the melt by preferential breaking of Si-O-Si bonds of the most polymerized tetrahedral sites, mainly Q4.  相似文献   

12.
The structure of silicate melts in the system Na2O·4SiO2 saturated with reduced C-O-H volatile components and of coexisting silicate-saturated C-O-H solutions has been determined in a hydrothermal diamond anvil cell (HDAC) by using confocal microRaman and FTIR spectroscopy as structural probes. The experiments were conducted in-situ with the melt and fluid at high temperature (up to 800 °C) and pressure (up to 1435 MPa). Redox conditions in the HDAC were controlled with the reaction, Mo + H2O = MoO2 + H2, which is slightly more reducing than the Fe + H2O = FeO + H2 buffer at 800 °C and less.The dominant species in the fluid are CH4 + H2O together with minor amounts of molecular H2 and an undersaturated hydrocarbon species. In coexisting melt, CH3 - groups linked to the silicate melt structure via Si-O-CH3 bonding may dominate and possibly coexists with molecular CH4. The abundance ratio of CH3 - groups in melts relative to CH4 in fluids increases from 0.01 to 0.07 between 500 and 800 °C. Carbon-bearing species in melts were not detected at temperatures and pressures below 400 °C and 730 MPa, respectively. A schematic solution mechanism is, Si-O-Si + CH4?Si-O-CH3+H-O-Si. This mechanism causes depolymerization of silicate melts. Solution of reduced (C-O-H) components will, therefore, affect melt properties in a manner resembling dissolved H2O.  相似文献   

13.
Hydrothermal experiments were conducted to determine the partitioning of Cl between rhyolitic to rhyodacitic melts, apatite, and aqueous fluid(s) and the partitioning of F between apatite and these melts at ca. 200 MPa and 900-924 °C. The number of fluid phases in our experiments is unknown; they may have involved a single fluid or vapor plus saline liquid. The partitioning behavior of Cl between apatite and melt is non-Nernstian and is a complex function of melt composition and the Cl concentration of the system. Values of DClapat/melt (wt. fraction of: Cl in apatite/Cl in melt) vary from 1 to 4.5 and are largest when the Cl concentrations of the melt are at or near the Cl-saturation value of the melt. The Cl-saturation concentrations of silicate melts are lowest in evolved, silica-rich melts, so with elevated Cl concentrations in a system and with all else equal, the maximum values of DClapat/melt occur with the most felsic melt. In contrast, values of DFapat/melt range from 11 to 40 for these felsic melts, and many of these are an order of magnitude greater than those applying to basaltic melts at 200 MPa and 1066-1150 °C. The Cl concentration of apatite is a simple and linear function of the concentration of Cl in fluid. Values of DClfluid/apat for these experiments range from 9 to 43, and some values are an order of magnitude greater than those determined in 200-MPa experiments involving basaltic melts at 1066-1150 °C.In order to determine the concentrations and interpret the behavior of volatile components in magmas, the experimental data have been applied to the halogen concentrations of apatite grains from chemically evolved rocks of Augustine volcano, Alaska; Krakatau volcano, Indonesia; Mt. Pinatubo, Philippines; Mt. St. Helens, Washington; Mt. Mazama, Oregon; Lascar volcano, Chile; Santorini volcano, Greece, and the Bishop Tuff, California. The F concentrations of these magmas estimated from apatite-melt equilibria range from 0.06 to 0.12 wt% and are generally equivalent to the concentrations of F determined in the melt inclusions. In contrast, the Cl concentrations of the magmas estimated from apatite-melt equilibria (e.g., ca. 0.3-0.9 wt%) greatly exceed those determined in the melt inclusions from all of these volcanic systems except for the Bishop Tuff where the agreement is good. This discrepancy in estimated Cl concentrations of melt could result from several processes, including the hypothesis that the composition of apatite represents a comparatively Cl-enriched stage of magma evolution that precedes melt inclusion entrapment prior to the sequestration of Cl by coexisting magmatic aqueous and/or saline fluid(s).  相似文献   

14.
SHRIMP zircon U-Pb dates, combined with in-situ Hf isotopic data, provide new constraints on the petrogenesis and protolith of peralkaline, metaluminous and peraluminous intrusions and rhyolitic tuffs in the Emeishan large igneous province, with significant bearing on crustal melting associated with mantle plumes. Syenite and A-type granitic intrusions from Huili, Miyi and Taihe in the center of this large igneous province yield U-Pb dates at ∼260 Ma, consistent with the ages obtained for mafic layered intrusions in the same province. Zircon from these rocks exhibits a wide range of initial Hf isotope ratios (εHf(t) = −1.4 to +13.4), with corresponding TDM1 of 400-900 Ma. The highest εHf(t) value is only marginally lower than that of depleted mantle reservoir at 260 Ma, suggesting that their source is primarily juvenile crust added during Emeishan volcanism, with incorporation of variable amounts of Neoproterozoic crust. The trigger of crustal melting is most likely related to advective heating associated with magmatic underplating. In contrast, the 255-251 Ma peraluminous granites from Ailanghe and 238 Ma rhyolitic tuff from Binchuan, have negative initial εHf values of −1.3 to −4.4, and of −7.7 to −14, respectively. Hf isotopic model ages and presence of inherited zircons indicate their derivation from Mesoproterozoic and Paleoproterozoic crust, respectively. Given the time lag relative to the plume impact (∼260 Ma) and insignificant mantle contribution to 255-238 Ma magmatism, conductive heating is suggested as the trigger of crustal melting that resulted in formation of delayed felsic magmas. The involvement of older crust in younger felsic magmas is consistent with upward heat transfer to the lithosphere during plume impregnation, if the age of crust is inversely stratified, i.e., changes from Paleoproterozoic to Mesoproterozoic to Neoproterozoic to Permian with increasing depth. Such crust may have resulted from episodic, downward crustal growth during the evolution of the western Yangtze Craton.  相似文献   

15.
FTIR spectroscopy of OH in olivine: A new tool in kimberlite exploration   总被引：1，自引：0，他引：1  
Our study of olivines from Canadian kimberlites shows that the application of FTIR spectroscopy significantly improves the reliability of olivine as a kimberlite indicator mineral (KIM). We have developed an algorithm that yields the water concentration and the normalized intensity of the OH IR absorption band at 3572 cm−1 from unpolished olivine grains of unknown thickness. For 80% of kimberlitic olivines these two parameters are significantly higher than those for olivines from non-kimberlitic magmas and consequently, olivines with water concentrations >60 ppm and a strong absorption band at 3572 cm−1 can be reliably classified as being kimberlitic.We have identified two major spectral features in the OH absorption bands of kimberlitic olivines that allow for a more detailed classification: (a) the presence of three types of high-requency OH absorption bands (Group 1A, 1B and 1C) and (b) the proportion of low-frequency OH absorption bands (Group 2) relative to high-frequency bands (Group 1). Comparison of our results with experimental studies suggests that differences within Group 1 OH absorption bands are due to different pressures of crystallization or hydrogenation. The three identified types of Group 1 OH absorption bands approximately correspond to high (P > 2 GPa, Group 1A), moderate (2-1 GPa, Group 1B), and low (<1 GPa, Group 1C) pressures of hydrogenation. Group 2 OH IR absorption bands in olivines with NiO > 3500 ppm are interpreted to reflect olivine-orthopyroxene equilibria and hence are indicative of xenocrystic olivine derived from lherzolitic or harzburgitic mantle sources. Interaction of xenocrystic olivine with hydrous kimberlitic melts with low silica activity likely will cause a gradual increase in Group 1 absorption bands. Therefore, FTIR spectra of olivine can be used to obtain qualitative estimates of the duration of interaction between mantle material and a kimberlitic melt.In addition to applications in kimberlite and diamond exploration, FTIR spectra of olivine phenocrysts, combined with mineral chemical data, may also provide insights into kimberlite evolution. Our data suggest that in some instances the ascent of kimberlitic magmas could have been interrupted at or near the Moho, followed by olivine crystallization and exsolution of aqueous fluids.  相似文献   

16.
Interaction between slab-derived melt and mantle peridotite and the role of slab melt as a metasomatizing agent in the sub-arc mantle is being increasingly recognized. Adakite, the slab melt erupted on the surface, usually exhibits anomalously high MgO, CaO, Cr and Ni contents that indicate interaction with mantle peridotitite. Here we note that Cenozoic adakites have Na2O contents below 5.8 wt.% with ∼95% samples lower than 5.0 wt.%, and are generally depleted in this component relative to experimental basalt partial melts (mostly beyond 5.0 wt.% and up to 9.0 wt.% Na2O) produced under 1.5-3.0 GPa conditions that are most relevant to adakite production. We interpret the adakite Na depletion to be also a consequence of the melt / rock reaction that takes place within the hot mantle wedge. During ascent and reaction with mantle peridotite, primary adakite melts gain mantle components MgO, CaO, Cr and Ni but lose Na2O, SiO2 and perhaps K2O to the mantle, leading to Na-rich mantle metasomatism. Selective assimilation of predominately mantle clinopyroxene, some spinel and minor olivine at high T/P has been considered to be an important process in producing high-Mg adakites from primary low-Mg slab melts [Killian, R., Stern, C. R., 2002. Constraints on the interaction between slab melts and the mantle wedge from adakitic glass in peridotite xenoliths. Eur. J. Mineral. 14, 25-36]. In such a process, Na depletion in the assimilated melt is the result of dilution due to the increase in melt mass. Phase relationships in the reaction system siliceous melt + peridotite and quantitative calculation suggest that assimilation of mantle clinopyroxene, olivine and spinel and fractional crystallization of sodic amphibole and orthopyroxene, under conditions of moderate T/P and increasing melt mass, is also an important process that modifies the composition of adakites and causes the Na depletion.  相似文献   

17.
We have performed a series of molecular dynamics simulations aimed at the evaluation of the solubility of CO2 in silicate melts of natural composition (from felsic to ultramafic). In making in contact within the simulation cell a supercritical CO2 phase with a silicate melt of a given composition, we have been able to evaluate (i) the solubility of CO2 in the P-T range 1473-2273 K and 20-150 kbar, (ii) the density change experienced by the CO2-bearing melt, (iii) the respective concentrations of CO2 and species in the melt, (iv) the lifetime and the diffusivity of these species and (v) the structure of the melt around the carbonate groups. The main results are the following:(1) The solubility of CO2 increases markedly with the pressure in the three investigated melts (a rhyolite, a mid-ocean ridge basalt and a kimberlite) from about ∼2 wt% CO2 at 20 kbar to ∼25 wt% at 100 kbar and 2273 K. The solubility is found to be weakly dependent on the melt composition (as far as the present compositions are concerned) and it is only at very high pressure (above ∼100 kbar) that a clear hierarchy between solubilities occurs (rhyolite < MORB < kimberlite). Furthermore at a given pressure the calculated solubility is negatively correlated with the temperature.(2) In CO2-saturated melts, the proportion of carbonate ions is positively correlated with the pressure at isothermal condition and is negatively correlated with the temperature at isobaric condition (and vice versa for molecular CO2). Furthermore, at fixed (P, T) conditions the proportion of carbonate ions is higher in CO2-undersaturated melts than in the CO2-saturated melt. Although the proportion of molecular CO2 decreases when the degree of depolymerization of the melt increases, it is still significant in CO2-saturated basic and ultrabasic compositions at high temperatures. This finding is at variance with experimental data on CO2-bearing glasses which show no evidence of molecular CO2 as soon as the degree of depolymerization of the melt is high (e.g. basalt). These conflicting results can be reconciled with each other by noticing that a simple low temperature extrapolation of the simulation data predicts that the proportion of molecular CO2 in basaltic melts might be negligible in the glass at room temperature.(3) The carbonate ions are found to be transient species in the liquid phase, with a lifetime increasing exponentially with the inverse of the temperature. Contrarily to a usual assumption, the diffusivity of carbonate ions into the liquid silicate is not vanishingly small with respect to that of CO2 molecules: in MORB they differ from each other by a factor of ∼6 at 1473 K and only a factor of ∼2 at 2273 K. Although the bulk diffusivity of CO2 is governed primarily by the diffusivity of CO2 molecules, the carbonate ions contribute significantly to the diffusivity of CO2 in depolymerized melts.(4) Concerning the structure of the CO2-bearing silicate melt, the carbonate ions are found to be preferentially associated with NBO’s of the melt, with an affinity for NBOs which exceeds that for BOs by almost one order of magnitude. This result explains why the concentration in carbonate ions is positively correlated with the degree of depolymerization of the melt and diminishes drastically in fully polymerized melts where the number of NBO’s is close to zero. Furthermore, the network modifier cations are not randomly distributed in the close vicinity of carbonate groups but exhibit a preferential ordering which depends at once on the nature of the cation and on the melt composition. However at the high temperatures investigated here, there is no evidence of long lived complexes between carbonate groups and metal cations.  相似文献   

18.
Dunite, wehrlite and websterite are rare members of the mantle xenolith suite in the Kimberley kimberlites of the Kaapvaal Craton in southern Africa. All three types were originally residues of extensive melt extraction and experienced varying amounts and types of melt re-enrichment. The melt depletion event, dated by Re-Os isotope systematics at 2.9 Ga or older, is evidenced by the high Mg# (Mg/(Mg + Fe)) of silicate minerals (olivine (0.89-0.93); pyroxene (0.88-0.93); garnet (0.72-0.85)), high Cr# (Cr/(Cr + Al)) of spinel (0.53-0.84) and mostly low whole-rock SiO2, CaO and Al2O3 contents. Shortly after melt depletion, websterites were formed by reaction between depleted peridotites and silica-rich melt (>60 wt% SiO2) derived by partial melting of eclogite before or during cratonization. The melt-peridotite interaction converted olivine into orthopyroxene.All three xenolith types have secondary metasomatic clinopyroxene and garnet, which occur along olivine grain boundaries and have an amoeboid texture. As indicated by the preservation of oxygen isotope disequilibrium in the minerals and trace-element concentrations in clinopyroxene and garnet, this metasomatic event is probably of Mesozoic age and was caused by percolating alkaline basaltic melts. This melt metasomatism enriched the xenoliths in CaO, Al2O3, FeO and high-field-strength-elements, and might correspond to the Karoo magmatism at 200 Ma. The websterite xenoliths experienced both the orthoyproxene-enrichment and clinopyroxene-garnet metasomatic events, whereas dunite and wehrlite xenoliths only saw the later basaltic melt event, and may have been situated further away from the source of melt migration channels.  相似文献   

19.
Lavas from the island of São Miguel, Azores Archipelago have long been known to display large radiogenic isotopic variability, that ranges from “depleted” isotopic signatures (e.g. high εNd ∼ +5) in the west, typical of many ocean island basalts, to more “enriched” compositions (e.g. low εNd ∼ +1) in the east. Here, we further characterise the geochemistry of lavas from this remarkable locality, focussing on the nature and origin of the enriched source. Our new isotope data define a striking, linear array in Nd and Hf isotope space that points towards an unusual, enriched composition below the mantle array. This distinctive Hf-Nd isotope signature is associated with elevated values of all three radiogenic Pb isotope ratios. Although the enriched component has certain geochemical similarities to both terrigenous sediments and some samples of the continental mantle lithosphere, such comparisons do not stand closer examination. In the absence of a clear, modern analogue we explore the isotope evolution of some simple, model melt compositions to investigate plausible means of producing an appropriate enriched component. Nd-Hf isotope characteristics provide the tightest constraints and can be reproduced by an ancient (∼3 Ga), modest-degree melt (∼2%) from a garnet peridotite source. Currently, modest-degree melts from garnet-bearing sources are found forming some major oceanic islands. Subduction, isolation and later mixing of small amounts (<5%) of such basaltic material with more ubiquitous ambient mantle can account for the isotopic characteristics of the enriched São Miguel source. Yet the incompatible element ratios of the enriched São Miguel lavas do not show “recycled” signatures of near-surface alteration nor subduction zone dehydration. Thus, we infer that the enriched component was originally under-plated basalt, intruded into oceanic mantle lithosphere rather than forming the island edifice itself. Since the extreme isotope compositions of São Miguel reflect unextraordinary, albeit ancient, magmatic fractionation, the general rarity of such signatures indicates the efficiency of mantle processes in homogenising or hiding similar sources.  相似文献   

20.
The sulfur concentration at pyrrhotite- and anhydrite-saturation in primitive hydrous basaltic melt of the 2001-2002 eruption of Mt. Etna was determined at 200 MPa, T = 1050-1250 °C and at log fO2 from FMQ to FMQ+2.2 (FMQ is Fayalite-Magnetite-Quartz oxygen buffer). At 1050 °C Au sample containers were used. A double-capsule technique, using a single crystal olivine sample container closed with an olivine piston, embedded in a sealed Au80Pd20 capsule, was developed to perform experiments in S-bearing hydrous basaltic systems at T > 1050 °C. Pyrrhotite is found to be a stable phase coexisting with melt at FMQ-FMQ+0.3, whereas anhydrite is stable at FMQ+1.4-FMQ+2.2. The S concentration in the melt increases almost linearly from 0.12 ± 0.01 to 0.39 ± 0.02 wt.% S at FeS-saturation and from 0.74 ± 0.01 to 1.08 ± 0.04 wt.% S at anhydrite-saturation with T ranging from 1050-1250 °C. The relationships between S concentration at pyrrhotite and/or anhydrite saturation, MgO content of the olivine-saturated melt, T, and log fO2 observed in this study and from previous data are used to develop an empirical model for estimating the magmatic T and fO2 from the S and MgO concentrations of H2O-bearing olivine-saturated basaltic melts. The model can also be used to determine maximum S concentrations, if fO2 and MgO content of the melt are known. The application of the model to compositions of melt inclusions in olivines from Mt. Etna indicates that the most primitive magmas trapped in inclusions might have been stored at log fO2 slightly higher than FMQ+1 and at T = 1100-1150 °C, whereas more evolved melts could have been trapped at T ? 1100 °C. These values are in a good agreement with the estimates obtained by other independent methods reported in the literature.  相似文献   

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