Sulfur radical species form gold deposits on Earth

被引:143
作者
Pokrovski, Gleb S. [1 ]
Kokh, Maria A. [1 ]
Guillaume, Damien [1 ]
Borisova, Anastassia Y. [1 ]
Gisquet, Pascal [1 ]
Hazemann, Jean-Louis [2 ]
Lahera, Eric [3 ]
Del Net, William [3 ]
Proux, Olivier [3 ]
Testemale, Denis [2 ]
Haigis, Volker [4 ,5 ,6 ]
Jonchiere, Romain [4 ,5 ,6 ]
Seitsonen, Ari P. [4 ]
Ferlat, Guillaume [5 ,6 ]
Vuilleumier, Rodolphe [4 ]
Saitta, Antonino Marco [5 ,6 ]
Boiron, Marie-Christine [7 ]
Dubessy, Jean [7 ]
机构
[1] Univ Toulouse, Grp Metallogenie Expt, Observ Midi Pyrenees, GET,CNRS,IRD, F-31400 Toulouse, France
[2] Univ Grenoble Alpes, Inst NEEL, CNRS, F-38042 Grenoble, France
[3] Univ Grenoble Alpes, Observ Sci Univers Grenoble, F-38400 St Martin Dheres, France
[4] Univ Paris 06, PSL Res Univ, Sorbonne Univ, Ecole Normale Super,Dept Chim,CNRS,UMR Pasteur 8, F-75005 Paris, France
[5] Univ Paris 06, Sorbonne Univ, F-75005 Paris, France
[6] IMPMC, F-75005 Paris, France
[7] Univ Lorraine, CNRS, Ctr Rech Geol Mat Premieres Minerales & Energet C, GeoRessources, F-54506 Vandoeuvre Les Nancy, France
关键词
gold; sulfur; ore deposit; hydrothermal fluid; trisulfur ion; HYDROTHERMAL FLUIDS; GEOLOGICAL FLUIDS; METAL BUDGET; ORE-DEPOSITS; CARLIN-TYPE; S-3(-) ION; TRANSPORT; PORPHYRY; COMPLEXES; COPPER;
D O I
10.1073/pnas.1506378112
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Current models of the formation and distribution of gold deposits on Earth are based on the long-standing paradigm that hydrogen sulfide and chloride are the ligands responsible for gold mobilization and precipitation by fluids across the lithosphere. Here we challenge this view by demonstrating, using in situ X-ray absorption spectroscopy and solubility measurements, coupled with molecular dynamics and thermodynamic simulations, that sulfur radical species, such as the trisulfur ion S-3(-), form very stable and soluble complexes with Au+ in aqueous solution at elevated temperatures (>250 degrees C) and pressures (>100 bar). These species enable extraction, transport, and focused precipitation of gold by sulfur-rich fluids 10-100 times more efficiently than sulfide and chloride only. As a result, S-3(-) exerts an important control on the source, concentration, and distribution of gold in its major economic deposits from magmatic, hydrothermal, and metamorphic settings. The growth and decay of S-3(-) during the fluid generation and evolution is one of the key factors that determine the fate of gold in the lithosphere.
引用
收藏
页码:13484 / 13489
页数:6
相关论文
共 48 条
[1]  
Barnes HL, 1997, GEOCHEMISTRY HYDROTH
[2]   Mixing of metamorphic and surficial fluids during the uplift of the Hercynian upper crust: consequences for gold deposition [J].
Boiron, MC ;
Cathelineau, M ;
Banks, DA ;
Fourcade, S ;
Vallance, J .
CHEMICAL GEOLOGY, 2003, 194 (1-3) :119-141
[3]   High gold concentrations in sulphide-bearing magma under oxidizing conditions [J].
Botcharnikov, Roman E. ;
Linnen, Robert L. ;
Wilke, Max ;
Holtz, Francois ;
Jugo, Pedro J. ;
Berndt, Jasper .
NATURE GEOSCIENCE, 2011, 4 (02) :112-115
[4]   HYDROTHERMAL TRANSPORT AND DEPOSITION OF GOLD [J].
BOYLE, RW .
ECONOMIC GEOLOGY, 1969, 64 (01) :112-&
[5]   Ubiquitous trisulfur radical anion: fundamentals and applications in materials science, electrochemistry, analytical chemistry and geochemistry [J].
Chivers, Tristram ;
Elder, Philip J. W. .
CHEMICAL SOCIETY REVIEWS, 2013, 42 (14) :5996-6005
[6]  
Cotton F.A., 1999, Advanced Inorganic Chemistry
[7]   Earth's continental crustal gold endowment [J].
Frimmel, H. E. .
EARTH AND PLANETARY SCIENCE LETTERS, 2008, 267 (1-2) :45-55
[8]  
Garofalo PS, 2014, GEOL SOC SPEC PUBL, V402, P71, DOI 10.1144/SP402.8
[9]   100th Anniversary Special Paper:: Secular changes in global tectonic processes and their influence on the temporal distribution of gold-bearing mineral deposits [J].
Groves, DI ;
Condie, KC ;
Goldfarb, RJ ;
Hronsky, JMA ;
Vielreicher, RM .
ECONOMIC GEOLOGY, 2005, 100 (02) :203-224
[10]   THE ROLE OF MAGMAS IN THE FORMATION OF HYDROTHERMAL ORE-DEPOSITS [J].
HEDENQUIST, JW ;
LOWENSTERN, JB .
NATURE, 1994, 370 (6490) :519-527