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In situ observations of liquid-liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 degrees C: Implications for Zn2+-SO42- association and evolution of submarine hydrothermal fluids
Wang, Xiaolin1,2; Wan, Ye1; Hu, Wenxuan1,2; Chou, I-Ming3; Cao, Jian1,2; Wang, Xiaoyu1; Wang, Meng4; Li, Zhen5
2016-05-15
Source PublicationGEOCHIMICA ET COSMOCHIMICA ACTA
Volume181Pages:126-143
AbstractLiquid-liquid immiscibility is gaining recognition as an important process in hydrothermal fluid activity. However, studies of this complex process are relatively limited. We examined liquid-liquid immiscibility in aqueous ZnSO4 solutions at temperatures above similar to 266.5 degrees C and at vapor-saturation pressures. The homogeneous aqueous ZnSO4 solution separated into ZnSO4-rich (L1) and ZnSO4-poor (L2) liquid phases coexisting with the vapor phase. The L1-L2 phase separation temperature decreased with increasing ZnSO4 concentration up to 1.0 mol/kg, and then increased at greater ZnSO4 concentrations, showing a typical lower critical solution temperature (LCST) of similar to 266.5 degrees C. Gunningite (ZnSO4 center dot H2O) precipitated in 2.0 mol/kg ZnSO4 solution at 360 degrees C. The L1-L2 phase separation resulted mainly from the strong Zn2+-SO42- association at high temperatures. The major results of this study are: (1) the discovery of the LCST in these systems, a macroscale property associated with polymeric mixtures; (2) analyses of the peak area ratios of the nu(1)(SO42-) and OH stretching bands, which suggest that the sulfate concentration increases with increasing temperature in L1, especially above 375 degrees C; (3) a new Raman nu(1)(SO42-) mode at similar to 1005 cm(-1) observed only in the L1 phase, whose fraction increases with increasing temperature; and (4) the shape of the OH Raman stretching band, which indicates that water molecules and solute interact much more strongly in L1 than in the coexisting L2 phase, suggesting that water molecules fit into the framework formed by various Zn2+-SO42- pairs and chain structures in L1. These results have potential implications for understanding transport and reduction of seawater-derived sulfate in submarine hydrothermal systems. The formation of an immiscible sulfate-rich liquid phase can favor the circulation of sulfate within mid-ocean ridge basalt because the sulfate-rich liquid density is higher than that of the coexisting fluid. The reduction of sulfate could also be accelerated because sulfate is locally concentrated and strong Zn2+-SO42- association increases the reactivity of sulfate. (C) 2016 Elsevier Ltd. All rights reserved.
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
DOI10.1016/j.gca.2016.03.001
Indexed BySCI
Language英语
WOS KeywordJUAN-DE-FUCA ; SULFUR ISOTOPIC COMPOSITION ; EAST PACIFIC RISE ; EQUATION-OF-STATE ; X-RAY-DIFFRACTION ; MODERN SEA-FLOOR ; RAMAN-SPECTROSCOPY ; VENT FLUIDS ; ION-ASSOCIATION ; SULFATE ION
WOS SubjectGeochemistry & Geophysics
WOS IDWOS:000373618200008
Citation statistics
Cited Times:11[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Version预印本
Identifierhttp://ir.idsse.ac.cn/handle/183446/1563
Collection深海科学研究部_深海极端环境模拟研究实验室
Corresponding AuthorWang, Xiaolin
Affiliation1.Nanjing Univ, Sch Earth Sci & Engn, State Key Lab Mineral Deposits Res, Nanjing 210023, Jiangsu, Peoples R China
2.Nanjing Univ, Inst Energy Sci, Nanjing 210023, Jiangsu, Peoples R China
3.Chinese Acad Sci, Sanya Inst Deep Sea Sci & Engn, Lab Expt Study Deep Sea Extreme Condit, Sanya 572000, Hainan, Peoples R China
4.East China Mineral Explorat & Dev Bur, Nanjing 210007, Jiangsu, Peoples R China
5.Curtin Univ, Dept Appl Geol, Perth, WA 6845, Australia
Recommended Citation
GB/T 7714
Wang, Xiaolin,Wan, Ye,Hu, Wenxuan,et al. In situ observations of liquid-liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 degrees C: Implications for Zn2+-SO42- association and evolution of submarine hydrothermal fluids[J]. GEOCHIMICA ET COSMOCHIMICA ACTA,2016,181:126-143.
APA Wang, Xiaolin.,Wan, Ye.,Hu, Wenxuan.,Chou, I-Ming.,Cao, Jian.,...&Li, Zhen.(2016).In situ observations of liquid-liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 degrees C: Implications for Zn2+-SO42- association and evolution of submarine hydrothermal fluids.GEOCHIMICA ET COSMOCHIMICA ACTA,181,126-143.
MLA Wang, Xiaolin,et al."In situ observations of liquid-liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 degrees C: Implications for Zn2+-SO42- association and evolution of submarine hydrothermal fluids".GEOCHIMICA ET COSMOCHIMICA ACTA 181(2016):126-143.
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