Influence of temperature, pressure, and fluid salinity on the distribution of chlorine into serpentine minerals

doi:10.1016/j.jseaes.2017.04.022

Journal of Asian Earth Sciences

Volume 145, Part A, 1 September 2017, Pages 101-110

https://doi.org/10.1016/j.jseaes.2017.04.022 Get rights and content

Highlights

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The incorporation of chlorine into serpentine was experimentally studied.
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Temperature, pressure and fluid salinity greatly influence chlorine behavior.
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Chlorine in serpentine reached maximum at 200 °C, which decreased at 300–500 °C.
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Chlorine behavior is closely associated with the mobility of aluminum and silica.
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Serpentine is an important carrier of chlorine in subduction zones.

Abstract

Serpentinization produces serpentine minerals that have abundant water and fluid-mobile elements (e.g., Ba, Cs, and Cl). The dehydration of serpentine minerals produces chlorine-rich fluids that may be linked with the genesis of arc magmas. However, the factors that control the distribution of chlorine into serpentine minerals remain poorly constrained. We performed serpentinization experiments at 80–500 °C and pressures from vapor saturated pressures to 20 kbar on peridotite, orthopyroxene, and olivine with <5% pyroxene. The results show that the concentrations of chlorine in serpentine minerals were up to 1.2 wt% at 200 °C, whereas they decreased slightly at 311–400 °C and 3.0 kbar and became significantly lower at 485 °C and 3.0 kbar, ∼0.1 wt%. Fluid salinity greatly decreased chlorine concentrations of olivine-derived serpentine produced at 400 °C and 3.0 kbar, which was associated with a decrease in silica mobility during serpentinization. By contrast, influence of fluid salinity at 311 °C and 3.0 kbar is minor. Moreover, chlorine distribution into serpentine can be influenced by primary minerals of serpentine. Serpentine formed in olivine-only experiments at 311 °C and 3.0 kbar had 0.08 ± 0.03 wt% Cl, which is significantly lower than chlorine concentrations of serpentine minerals (0.49 ± 0.36 wt%) produced in orthopyroxene-only experiments. By contrast, for experiments at 311 °C and 3.0 kbar, olivine- and orthopyroxene-derived serpentine had comparable amounts of chlorine. In particular, olivine-derived serpentine had 0.16 ± 0.09 wt% Cl that was slightly higher than chlorine concentrations of serpentine formed in olivine-only experiments, whereas orthopyroxene-derived serpentine had significantly lower chlorine concentrations than that formed in orthopyroxene-only experiments. The contrast may be associated with releases of aluminum and silica from pyroxene minerals, which possibly results in a decrease in chlorine concentrations of serpentine. The concentrations of chlorine in serpentine formed in experiments at 311 °C and 3.0 kbar were slightly lower than those in serpentine produced at 300 °C and 8.0 kbar, which may be associated with influence of pressure on the mobility of iron and silica. The experimental results of this study indicate that serpentine minerals are important carriers of chlorine in subduction zones. It also suggests that chlorine is significant for the redistribution of cations during serpentinization.

Introduction

Serpentinization, a hydrothermal alteration of ultramafic rocks (typically peridotite and komatiite) at relatively low temperatures (≤500 °C), produces serpentine minerals, (±) brucite, (±) talc, and (±) magnetite. Serpentinization occurs at various geological settings, including the ocean floor, mid-ocean ridges, and subduction zones (e.g., Charlou et al., 1996, Charlou et al., 2000, Maekawa et al., 2001, Hyndman and Peacock, 2003, Mével, 2003, Evans et al., 2013). Serpentinization greatly modifies chemical and physical properties of the oceanic lithosphere (e.g., Escartín et al., 1997, Escartín et al., 2001, Scambelluri et al., 1995, Mével, 2003, Guillot and Hattori, 2013). Serpentinites (with >90% serpentine) have a dramatically lower density compared to primary peridotites, whereas serpentinites have magnetic susceptibility around one to two orders of magnitude higher (Mével, 2003, Evans et al., 2013). As suggested by deformation experiments, a very low degree of serpentinization can greatly decrease the strength of olivine (Escartín et al., 1997, Escartín et al., 2001). Analyses of natural serpentinites show that serpentine minerals can incorporate not only water (up to 13.5 wt%) but also chlorine and fluid-mobile elements, such as Cs, Ba, and Sr (Scambelluri et al., 1995, Hattori and Guillot, 2003, Deschamps et al., 2012, Guillot and Hattori, 2013). Compared to fresh peridotite (with <30 ppm Cl), serpentinites have around one to two orders of magnitude higher chlorine (e.g., Bonifacie et al., 2008, Barnes and Straub, 2010). Thermodynamic and experimental studies suggest that serpentine minerals can be stable at depths of greater than 200 km (Ulmer and Trommsdorff, 1995, Schmidt and Poli, 1998). Therefore, serpentinization may play a significant role for the transfer of H₂O, chlorine, and fluid-mobile elements into the mantle.

In spite of the importance, the mechanisms that control the incorporation of chlorine into serpentine minerals still remain poorly understood (Rucklidge, 1972, Rucklidge and Patterson, 1977, Anselmi et al., 2000, Scambelluri et al., 2004, Sharp and Barnes, 2004, Barnes and Sharp, 2006, Bonifacie et al., 2008). Chlorine can be hosted in a structurally-bound site, i.e., substitute for the hydroxyl group in serpentine (e.g., Anselmi et al., 2000) or in a water-soluble site (e.g., Rucklidge and Patterson, 1977, Sharp and Barnes, 2004, Barnes and Sharp, 2006). Hydrothermal experiments show that chlorine in the water-soluble site is readily leached by water (Sharp and Barnes, 2004, Barnes and Sharp, 2006). Fluid inclusions of natural serpentinites commonly have salinities with great variations (e.g., Philippot et al., 1998, Scambelluri et al., 1997, Scambelluri et al., 2004). As a consequence, chlorine in serpentine may vary greatly even under the same T-P conditions. Analyses of natural serpentinites show that oceanic serpentinites, possibly formed at ∼250 °C, had abundant chlorine, up to 0.62 wt%, whereas antigorite serpentinites with the experience of eclogite-facies metamorphic grade contained much less chlorine (Scambelluri et al., 2004). However, natural serpentinites commonly experience multistage metamorphic history, and consequently the chlorine may not necessarily represent a single T-P condition. In particular, chlorine in natural serpentinites may be greatly influenced by lateral metamorphic fluids. Therefore, it is necessary to experimentally investigate the influence of temperature, pressure, and salinity of starting fluids on the incorporation of chlorine into serpentine minerals.

In this study, we performed experiments at 80–500 °C and pressures ranging from vapor saturated pressures to 20 kbar with peridotite, orthopyroxene, and olivine with <5% pyroxene as starting materials. The objectives are to (1) quantify the concentrations of chlorine in serpentine formed under different conditions, (2) investigate influence of temperature, pressure, fluid salinity, and water/rock ratios on chlorine distribution into serpentine minerals, and (3) assess the importance of serpentinization for the recycling of chlorine in subduction zones.

Section snippets

Preparation of starting materials

An unaltered peridotite, sampled at Panshishan (Jiangsu Province, China) where it occurs as xenoliths in alkaline basalts (Chen et al., 1994, Sun et al., 1998, Xu et al., 2008, Yang, 2008), was taken as the starting material. Peridotite is composed of ∼65 vol% olivine, 20 vol% orthopyroxene, 15 vol% clinopyroxene and ∼2 vol% spinel. Chemical compositions of primary minerals in peridotite were described in a previous experimental study (Huang et al., 2015a). The peridotite is fresh, as evidenced by

Identification of secondary hydrous minerals

As revealed by SEM imaging and Fourier transform infrared spectroscopy analyses (Fig. 1), the main secondary hydrous mineral produced at 311 °C and 3.0 kbar was fibrous chrysotile, and tabular shaped lizardite was formed in experiments at 80–200 °C and vapor saturated pressures, and at 400 °C and 3.0 kbar. Infrared spectra of solid products show typical infrared bands of serpentine at 954 cm⁻¹, 1087 cm⁻¹, and 3686 cm⁻¹. The bands at 954 cm⁻¹ and 1087 cm⁻¹ were assigned to the Si single bond O group of serpentine, and

Conclusions

Hydrothermal experiments were performed at 80–500 °C and pressures ranging from vapor saturated pressures to 20 kbar to study influence of temperature, fluid salinity, water/rock ratios, and pressure on chlorine distribution into serpentine minerals. The results show that chlorine is hosted in a structurally-bound site of serpentine, and it strongly depends on the mobility of iron, aluminum and silica during serpentinization. Chlorine concentrations of serpentine formed at 80 °C were very low,

Acknowledgements

This research was financially supported by the Natural Science Foundation of China (91328204, 41603060), postdoctoral Science Foundation of China (2015M570735, 2016T90805), the Strategic Priority Research Program of Chinese Academy of Sciences (XDB06030100), and the scientific research fund of the Second Institute of Oceanography, SOA (JG1405). We thank S. Jiang at South China University of Technology for the help during FTIR analyses.

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Citation Excerpt :
Nevertheless, in peridotite experiment (olivine + orthopyroxene assemblage), serpentine replacing olivine and orthopyroxene has similar Cl contents that could be explained by the release of Si and Al from orthopyroxene during serpentinization, leading thus to a decrease in Cl content (Huang et al., 2017). Cl concentrations measured on serpentine in replacement of olivine (635 ± 237 ppm; Table 1) and serpentine in replacement of orthopyroxene (668 ± 237 ppm; Table 1) agree with both published and experimental data (Bonifacie et al., 2008; Huang et al., 2017). Other sources of fluids present in the Kerguelen archipelago, such as river waters or thermal springs, may also have influenced the rocks.
The spinel harzburgites xenoliths from the Lac Michèle outcrop, Kerguelen archipelago (South Indian Ocean), have the particularity to show unique and unusual evidences of fluids circulation and especially of serpentinization. In this paper, in situ and whole-rock petrographic and geochemical data on a selection of variously serpentinized samples are presented and attest that several episodes of fluid-rock interaction occurred. Serpentinization processes affected notably and with variable degrees the spinel harzburgites leading to changes in their mineralogy and chemical compositions. Degree of serpentinization ranges from very slight (LOI < 3 wt% and Fe³⁺/Fe_tot < 0.1) to moderate (4 wt% < LOI < 6 wt% and 0.21 < Fe³⁺/Fe_tot < 0.33). Most serpentinized samples show a preferential petrographic direction of serpentinization, forming a subparallel serpentine network, which is sometimes intersected by serpentine veins. As a result, at least two serpentinization episodes were identified within the Lac Michèle samples, without any chemical differences between the two generations except for Cl content. This suggests very few chemical evolution of the system during serpentinization. Due to the significant amount of Cl measured in serpentine minerals (601 ppm on average), the nature of the fluids that interacted with the spinel harzburgites xenoliths during the serpentinization events can be hypothesized to be seawater-like or seawater-derived fluids.
Chlorine isotope fractionation during serpentinization and hydrothermal mineralization: A density functional theory study
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Because of the large-scale recycling of volatile chlorine from the interior to the surface of the Earth, it is possible to use the isotopic composition of this element (δ³⁷Cl) in serpentinite to study mantle-crust interactions in subduction zones. It is also possible to use chlorine isotopes to track the evolution of fluids (through fluid inclusions/minerals) in hydrothermal ore-forming systems. Here, we report the results of a study of equilibrium chlorine isotope fractionation during serpentinization and hydrothermal mineralization based on density functional theory (DFT) and ab initio molecular dynamics simulations (AIMD). The chlorine isotope fractionation between lizardite and brine under variable thermodynamic conditions is described by the relationship 1000lnα_{lizardite-fluid} = 0.4170 × (1000/T)²–0.0281 × (1000/T) + 0.0582, which yielded Δ³⁷Cl_{lizardite-fluid} values of +0.49 to +4.46‰, +0.41 to +0.59‰ and + 0.49 to +3.57‰ for conditions at the seafloor, in the mantle wedge and in subduction zones. As a proxy for the diversity of metal-chloride complexes in hydrothermal fluids, the stable configurations of ferrous chloride complexes were acquired from long trajectories of AIMD simulation. Using this information, the chlorine isotope fractionation between minerals (i.e., apatite-group minerals, muscovite, phlogopite, tremolite, lizardite, marialite and metal halides) and ore-forming fluid was estimated. The relatively large chlorine isotope fractionation (Δ³⁷Cl _{minerals-hydrothermal fluid} values from −1.99 to +2.18‰) might partly explain the large variation of δ³⁷Cl in individual fluid inclusions observed in hydrothermal ore deposits. Because of the limited chlorine isotope fractionation between apatite and hydrothermal fluid (i.e., Δ³⁷Cl _{apatite-ore-forming fluid} of 0.06‰–0.69‰), apatite-group minerals might be an alternative to fluid inclusions for constraining the origin and evolution of hydrothermal fluids using δ³⁷Cl values. The theoretical constraints provided in this paper will facilitate the use of chlorine isotopes in tracking the sources of chloride in subduction zones and the origin of mineralizing fluids in ore deposits.
Synthetic fluid inclusions XXIII. Effect of temperature and fluid composition on rates of serpentinization of olivine
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Malvoisin and Brunet (2014) used magnetization saturation as well as SEM and petrographic observations to determine the extent of reaction using sintered olivine cylinders with various porosities as a starting material. The wide range in reported reaction rates could also be due to the use of different starting materials, which have included synthetic forsterite (Martin and Fyfe, 1970; Wegner and Ernst, 1983) and natural olivine (Malvoisin et al. 2012; Lafay et al., 2012; Andreani et al., 2013; Ogasawara et al., 2013; McCollom et al. 2016; Huang et al., 2017a, 2017b). During synthesis of forsterite in the laboratory, H2O can be incorporated into the forsterite structure as OH− defects.
Serpentinization, i.e. the hydrothermal alteration of ultramafic rocks, is an important and ubiquitous geologic process that occurs at slow- and ultraslow-spreading mid-ocean ridges, magma-poor passive margins, and subduction zones. While serpentinization occurs over a wide temperature range and involves diverse fluid compositions, few experimental studies systematically examined the effects of temperature and fluid composition on the kinetics of serpentinization of olivine, and published rates diverge greatly. We present results of an experimental study using synthetic fluid inclusions in Mg-rich olivine as micro-batch reactors to monitor the effects of temperature (100–350 °C), fluid composition (H₂O-MgCl-NaCl, H₂O-NaCl, H₂O-MgCl), and total salinity on serpentinization rates of olivine under closed system conditions.
Petrographic observations and Raman analyses of the experimental run products revealed the alteration of olivine to produce serpentine minerals, brucite, and magnetite. The salinity of the aqueous fluid in the inclusions increased as H₂O was removed from the solution and incorporated into the hydrous product phases and served as a proxy for reaction progress. The fastest serpentinization rates were found at 250 °C in the presence of a seawater-like aqueous solution. This result further suggests that serpentinization of olivine is fastest at lower temperatures (∼250 °C) and shallower depths in the oceanic lithosphere than suggested by previous studies (∼300 °C). Moreover, our experiments show that serpentinization rates decrease by several orders of magnitude as salinity and the concentration of dissolved Mg increase. These effects may reconcile some of the differences observed when comparing results of previously published rates obtained from experiments involving fluids of different compositions. We constructed a quantitative model based on the principle of detailed balance to predict variations in serpentinization rates (J_±) from low temperatures to 320 °C. It suggests that at 25 °C, serpentinization rates are 4 to 5 orders of magnitude slower than at 250 °C. Moreover, the temperature dependence model has been coupled with the kinetic effects derived from experiments involving different fluid composition to calculate the amount of time required for serpentinization of olivine having different reactive surface areas. The model shows that between 200 and 300 °C serpentinization is fast on geologic timescales when rocks with large reactive surface areas interact with a seawater-like aqueous solution (complete serpentinization in days to decades).
In situ elemental and Sr-O isotopic studies on apatite from the Xu-Huai intrusion at the southern margin of the North China Craton: Implications for petrogenesis and metallogeny
2019, Chemical Geology
Apatite as an excellent tracer of the magmatic and metallogenic processes, can incorporate large amounts of trace elements sensitive to melting and/or ore-fluid evolution. This paper reports a combined study of in situ apatite geochemistry and whole-rock geochemistry for Early Cretaceous ore-bearing (Group I) and ore-barren porphyries (Group II) in the Liguo Fe-Cu-Au deposit for the deciphering of its petrogenesis and the control factors of mineralization. The apatite from both Group I and Group II is magmatic fluorapatite, characterized by Eu negative anomalies, an enrichment of LREEs, and a depletion of HREEs. Meanwhile, both groups have high Sr/Y and δEu, indicating porphyry adakitic characteristics in origin. Compared to isotopes of whole rocks, the variable ⁸⁷Sr/⁸⁶Sr (0.70250–0.71262) and δ¹⁸O (6.22–9.00) values of both groups of apatite imply contributions of mantle-, crust- and/or sediment-derived materials. Although Group I apatite and II apatite show some similar geochemical characteristics, Group I apatite precedes the crystallization of plagioclase with no Sr-(La/Yb)_N/(La/Sm)_N/(Sm/Yb)_N correlations, whereas Group II apatite coincides with plagioclase crystallization, displaying positive correlations. The geochemistry of the elements (δEu, δCe, MnO and V) of these apatite groups, which are sensitive to a redox state, shows high oxygen fugacity (between HM and NNO), and Group I apatite has systematically higher oxygen fugacity than Group II apatite. More importantly, these different trace elements and oxygen fugacity characteristics between Group I apatite and Group II apatite can be used as an indicator of mineralization, and allow the skarn Fe-Cu-Au mineralization range to be drawn for the first time. Furthermore, the estimated F and Cl contents of the host parent magma (F = 1300–2446 ppm, Cl = 140–4780 ppm) are higher than those in a primitive mantle and average continental crust, suggesting an enrichment process of F and Cl. According to the above adakitic characteristics, high oxygen fugacity, and high F and Cl contents, the Pacific Plate subduction may be the main dynamic mechanism of the diagenesis and mineralization found in Liguo.
Effect of saline fluids on chlorine incorporation in serpentine
2018, Solid Earth Sciences
Citation Excerpt :
These observations suggest that saline fluids greatly increase the incorporation of structurally-bound chlorine in serpentine. The mechanisms that control Cl incorporation into serpentine have been widely discussed (e.g., Rucklidge and Patterson, 1977; Anselmi et al., 2000; Sharp and Barnes, 2004; Bonifacie et al., 2008; Huang et al., 2017a). Based on observations that aqueous fluids equilibrated with serpentine have Fe: Cl = 2:1, it has been proposed that chlorine is hosted in serpentine as submicroscopic grains in the form of Fe2(OH)3Cl (Rucklidge and Patterson, 1977).
The incorporation of chlorine in serpentine minerals is crucial for the recycling of chlorine in subduction zones. Fluid inclusions of natural serpentinites have up to 50 wt% Cl, but effect of fluid salinity on chlorine distribution in serpentine minerals is poorly constrained. In this study, natural serpentinites (Lichi Melange, Taiwan) with starting grain sizes of 100–177 μm were equilibrated in saline solutions (2.93 wt%, 8.78 wt%, and 19.30 wt% NaCl) at ambient temperature and pressure for experimental duration from 18 to 43 days. The concentrations of chlorine in serpentine minerals were analyzed using electron microprobe with a detection limit of 33 ppm. Serpentine before experiments has very low chlorine, 0.017 ± 0.009 wt%. In contrast, serpentine equilibrated in saline solutions contains chlorine around three times higher, e.g., serpentine equilibrated in 2.93 wt% NaCl has 0.077 ± 0.033 wt% Cl after 18 days. The serpentine was re-equilibrated in pure water for around 24 h in order to testify chlorine is hosted in a weak-bound or structurally-bound position. For serpentine minerals equilibrated in low-salinity solutions (2.93 wt% and 8.78 wt% NaCl), they lost ∼40% of Cl after re-equilibrated in pure water. Despite such release, chlorine in serpentine minerals is still higher than that of serpentine before experiment, which indicates that saline solutions increase structurally-bound chlorine of serpentine minerals. This is more efficient for high-salinity solution (19.30 wt% NaCl), and chlorine in serpentine re-equilibrated in pure water is essentially the same as that of serpentine equilibrated in the saline solution. Our experimental results suggest that chlorine in serpentine can be greatly modified by saline fluids. The structurally-bound chlorine may not necessarily reflect the T-P information of natural serpentinites.
Introduction to the structures and processes of subduction zones
2017, Journal of Asian Earth Sciences
Subduction zones have been the focus of many studies since the advent of plate tectonics in 1960s. Workings within subduction zones beneath volcanic arcs have been of particular interest because they prime the source of arc magmas. The results from magmatic products have been used to decipher the structures and processes of subduction zones. In doing so, many progresses have been made on modern oceanic subduction zones, but less progresses on ancient oceanic subduction zones. On the other hand, continental subduction zones have been studied since findings of coesite in metamorphic rocks of supracrustal origin in 1980s. It turns out that high-pressure to ultrahigh-pressure metamorphic rocks in collisional orogens provide a direct target to investigate the tectonism of subduction zones, whereas oceanic and continental arc volcanic rocks in accretionary orogens provide an indirect target to investigate the geochemistry of subduction zones. Nevertheless, metamorphic dehydration and partial melting at high-pressure to ultrahigh-pressure conditions are tectonically applicable to subduction zone processes at forearc to subarc depths, and crustal metasomatism is the physicochemical mechanism for geochemical transfer from the slab to the mantle in subduction channels. Taken together, these provide us with an excellent opportunity to find how the metamorphic, metasomatic and magmatic products are a function of the structures and processes in both oceanic and continental subduction zones. Because of the change in the thermal structures of subduction zones, different styles of metamorphism, metasomatism and magmatism are produced at convergent plate margins. In addition, juvenile and ancient crustal rocks have often suffered reworking in episodes independent of either accretionary or collisional orogeny, leading to continental rifting metamorphism and thus rifting orogeny for mountain building in intracontinental settings. This brings complexity to distinguish the syn-subduction processes and products from post-subduction processes and products. Nevertheless, available results indicate that our definition and understanding of subduction zone processes and products can be advanced by the convergence of observations and interpretations from geochemical, geological, geophysical and geodynamic studies of both oceanic and continental subduction zones. Therefore, insights into subduction zones can be provided by integration of different approaches from different targets in the near future.

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Full length ArticleInfluence of temperature, pressure, and fluid salinity on the distribution of chlorine into serpentine minerals

Highlights

Abstract

Introduction

Section snippets

Preparation of starting materials

Identification of secondary hydrous minerals

Conclusions

Acknowledgements

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Full length Article
Influence of temperature, pressure, and fluid salinity on the distribution of chlorine into serpentine minerals