Geology and pyrite sulfur isotopes of the Suoluogou gold deposit: Implication for crustal continuum model of orogenic gold deposit in northwestern margin of Yangtze Craton, SW China

Ore Geology Reviews 122 (2020) 103487

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Geology and pyrite sulfur isotopes of the Suoluogou gold deposit: Implication for crustal continuum model of orogenic gold deposit in northwestern margin of Yangtze Craton, SW China

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Panfei Sun, Qingfei Wang , Huajian Li, Chaoyi Dong, Jun Deng State Key Laboratory of Geological Processes and Mineral Resources, China University of Geosciences, Beijing 100083, China

A R T I C LE I N FO

A B S T R A C T

Keywords: Sulfur isotopes Subcrustal source Fluid evolution Crustal continuum model Suolougou gold deposit

Since the crustal continuum model was proposed mainly based on the variation of mineralization and alteration features of hypozonal, mesozonal, to epizonal deposits, genetic relationship between the different types in one ore belt still requires research. This issue was addressed by the research on the Suoluogou mesozonal orogenic gold deposit and its comparison with the hypozonal orogenic gold deposit in northwestern margin of Yangtze craton. Gold mineralization in Suoluogou is controlled by the bends of roughly EW-trending brittle fault developed in the Late Triassic strata, and it is associated with quartz, sericite, chlorite, carbonate, and sulfide alteration. Pyrite and arsenopyrite are the predominant sulfide mineral, with minor amounts of chalcopyrite, sphalerite, and galena. Four paragenetic stages are divided based on crosscutting relationship and mineral assemblage, including the pre-mineralization stage (stage Ⅰ), the hydrothermal quartz-sulfide stage (stage Ⅱ) and carbonate-quartz-sulfide stage (stage III), and the post-mineralization carbonate-pyrite stage (stage Ⅳ). The δ34S values for pyrite in stage Ⅱ vary from 6.01% to 8.59‰, and those in stage III are from 0.96% to 4.62‰. The decrease of δ34S value from stage Ⅱ to III is explained to the result of the isotope fractionation during separation of oxidised sulfur species in the brecciated space. The sulfide δ34S values in the initial gold mineralization stage of the Suoluogou deposit are similar to those of regional hypozonal orogenic deposit with derivation from metasomatized mantle in the craton margin. This similarity suggests that the mesozonal and hypozonal gold deposits formed in different depths of a crustal continuum model for the deposits sharing similar subcrustal source.

1. Introduction Orogenic gold deposits, widely distributed from Archean to Cenozoic, are a significant class of gold deposit accounting for an important part of global gold reserves (> 30%; Goldfarb et al., 2001; Groves et al., 1998). The orogenic gold deposits were classified into hypozonal, mesozonal and epizonal types based on the mineralization and alteration occurrence, and the different types were considered to constitute the crustal continuum model, a widely advocated model explaining the wide formation depths of orogenic gold deposits in the crust (Groves, 1993; Groves et al., 1998; Phillips and Powell, 2009). The hypozonal gold deposits occur mainly in Archean terranes (Groves, 1993; Knight et al., 1993), such as Challenger gold deposit in Southern Australia (Tomkins et al., 2004), Big Bell gold deposit in Western Australia (Phillips and Powell, 2009), and Consort deposit in South Africa (Dziggel et al., 2010). Compared with the hypozonal orogenic

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gold deposit, the mesozonal to epizonal orogenic gold deposits were much more widely developed (Groves, 1993; Groves et al., 1998; Wang et al., 2019b; Yang et al., 2015, 2016a; Zhang et al., 2019). The genetic relationship between hypozonal and mesozonal to epizonal orogenic gold deposits is critical to understanding the fluid sources and genesis of orgenic gold deposits, and also of great significance to the exploration of concealed gold deposits. Since the crustal continuum model was proposed, the genetic relationship among the different types of gold deposits still require more research for one ore belt, to provide new evidence for the debated source of ore fluid and metal. Due to the complexity of reaction between hydrothermal and wallrock and the ambiguous explanation of ore geochemistry, the ore-forming fluid in orogenic gold deposits was debated mainly from mantle to metamorphic origin (Goldfarb and Groves, 2015; Groves and Santosh, 2016; Hronsky et al., 2012; Phillips and Powell, 2010; Wang et al., 2019a,b). It was traditionallly

Corresponding author. E-mail address: [email protected] (Q. Wang).

https://doi.org/10.1016/j.oregeorev.2020.103487 Received 11 November 2019; Received in revised form 10 March 2020; Accepted 20 March 2020 Available online 23 March 2020 0169-1368/ © 2020 Elsevier B.V. All rights reserved.

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Fig. 1. Geological map of the northwestern margin of Yangtze Craton and its adjacent the Garzê-Litang suture zone showing the main rock units, structures, and the locations of major gold deposits (Edited based on Yan et al., 2018; Zhao et al., 2018). Inset map indicates tectonic location of the geological map.

considered that the metamorphic fluid released during the transition from greenschist- to amphibolite-facies metamorphism in the midupper crust is responsible for the formation of orogenic gold deposit (Goldfarb and Groves, 2015; Groves et al., 2019; Powell et al., 1991; Tomkins, 2010). But this model is equivocal because it can hardly explain the orogenic gold deposits that formed long post-dating regional metamorphism and those occurred in amphibolite (Goldfarb et al., 2005; Goldfarb and Groves, 2015; Zhao et al., 2018). For these cases, the mantle fluid model, that is ore fluids were derived from devolatilization of subducted oceanic plate or reactivation of fertile mantle, was proposed (Goldfarb et al., 1998; Deng et al., 2003, 2015, 2020a,b; Wang et al., 2019a; Zhao et al., 2018). In the northwestern margin of the Yangtze Craton, an important tectonic and metallogenic belt in southwestern China, hosts a number of orogenic gold deposits, including Suoluogou, Danba, and Yanzigou (Hou et al., 2012; Li et al., 2007; Wang, 2000; Wang et al., 2020; Yan et al., 2018; Zhao et al., 2018; Zhao, 2019). The Danba deposit represents a rare Phanerozoic hypozonal orogenic gold deposit formed in amphibolite-facies metamorphic environment (Zhao et al., 2018). It was proposed that the ore fluid of Danba was derived from the metasomatized lithospheric mantle rather than the hosting rock sequences (Zhao et al., 2018; Wang et al., 2020). Compared with hypozonal orogenic gold deposits, the mesozonal to epizonal orogenic gold

deposits are more widely distributed in the northwestern margin of the Yangtze Craton. However, the genetic relationship between hypozonal and mesozonal to epizonal orogenic gold deposits is unclear. Therefore, we studied the source and evolution of the poorly-documented mesozonal Suoluogou gold deposit, which has important implications for establishment of the crustal continuum model for the craton margin. Gold is commonly transported as bi- or tri-sulfide complexe in most hydrothermal fluids (Loucks and Mavrogenes, 1999; Pokrovski et al., 2015). Therefore, it is the key to correctly characterize the nature of ore fluids and identify sulfur sources for understanding the formation of gold deposits (Hoefs, 1997; Ohmoto, 1997; Ohmoto, 1979; Seal, 2006). Orogenic gold deposits commonly have the wide range of δ34S signatures, which has been attributed to multiple source fluids (Goldfarb et al., 2005), isotope fractionation between H2S(aq) and bulk fluid (Buhn et al., 2012; Goldfarb and Groves, 2015), input of granitic magmas (Hagemann and Cassidy, 2000; Neumayr et al., 2008), phase separation (Rye, 1993), fluid-pressure fluctuations (Hodkiewicz et al., 2009), and/or fluid-rock interaction (Ohmoto, 1986; Sangster, 1992; Palin and Xu, 2000). In-situ sulfur isotope analysis, which has been used to accurately determine fine-scale sulfur isotopic variations of the sulfides, can avoid the influence of mixing of sulfides with different generation and genesis in the sample preparation and thus provide pivotal clues to fluid evolution, source of sulfur, and mineralizing processes 2

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Fig. 2. (a) Geological map and (b) representative cross-sections of the Suoluogou deposit (after SGMBRGST, 2010). (c) Schematic maps showing stress condition change and a spatial relationship between structure and mineralization.

Cenozoic shear action (Hou, 1993; Hou et al., 2004; Huan et al., 2013; Leng et al., 2014; Song et al., 2004; Wang et al., 2013; Zhang et al., 2015a). The Tangyang dome, associated with the Suoluogou deposit, is located in the northwestern part of the metamorphic core complex dome belt at the northwestern margin of the Yangtze Craton. The core of the dome comprises mainly quartz schist, sericite slate, and granitic mylonite of Ordovician (Zeng et al., 2019). Outward of the dome core are mainly slate and marble of Triassic, characterized by sub-greenschist to greenschist facies assemblages (Yan et al., 1997; Zeng et al., 2019).

(Bendall et al., 2006; Chang et al., 2008; Hou et al., 2016; Kesler et al., 2005; Ma et al., 2018). In present study, we reported geology and mineralization of the Suoluogou mesozonal gold deposit and the sulfur isotope data of pyrite in different paragenetic stages. The aim of this study is to clarify: (1) the orogenic nature of the gold deposit; (2) the isotopic variation and evolution of ore fluid; and (3) the source of ore fluid and the crustal continuum model in the northwestern margin of Yangtze Craton. 2. Regional geology

3. Deposit geology

The northwestern margin of the Yangtze Craton is bordered by the Songpan-Garzê accretionary complex and the southeastern part of the Garzê-Litang suture zone (GLS). The northwestern margin of the Yangtze Craton is characterized by a large-scale Mesozoic domal domain with extensive exposure of Neoproterozoic crystalline basement along the domal domain (Fig. 1; Chen and Wilson, 1996; Wallis et al., 2003). The evolution of the northwestern margin of the Yangtze Craton involved four main events: 1) Late Proterozoic oceanic crust subduction (Zhao and Zhou, 2008; Zhou et al., 2002, 2008; Deng and Wang, 2016); 2) Late Triassic compression, which results in the contact between the northwestern margin of the Yangtze Craton with the GLS; 3) Late Triassic to Early Jurassic domal extension; and 4) Cenozoic thrusting related to India-Asia collision (Hou and Cook, 2009). During this process, Danba and Yanzigou, reported as typical orogenic gold deposits, were formed along the margin of the domes (Zhao et al., 2018; Zhao, 2019). The GLS, on the west of the Yangtze Craton and on the east of the Yidun arc belt (Fig. 1; Burchfiel and Chen, 2012; Hou et al., 2003; Reid et al., 2005; Yang et al., 2012, 2014a,b), is mainly characterized by the development of ophiolite assemblages (Deng et al., 2014a,b; Mo et al., 1993; Zhong, 1998). The GLS has witnessed complex tectonic evolutions from oceanic consumption and collision on Late Triassic, post-orogenic extension during the Jurassic to Cretaceous, and

3.1. Geology of the deposit The Suoluogou gold deposit, located in the southeastern part of Tangyang dome, owns a pre-mining resource of 57 t Au (SGMBRGST, 2010). The ore district is covered by the Late Triassic Qugasi Formation, which consists of limestone, quartz sandstone and carbonaceous slate (Fig. 3e), as well as mafic volcanic rocks (Figs. 2 and 3d). The mafic volcanic rocks comprises the mafic tuff and basalt (Fig. 2). The structures include nealy EW-, NW-, SN-, and NE-trending fault systems. The orebodies are spatially related to the nearly EW-trending Fa fault, which is approximately 3500 m long and generally strikes 240–290° with dip angle of 60–80°, mainly developed along the interface between carbonaceous slate and mafic tuff (Fig. 2). The carbonaceous slate and mafic tuff are highly fractured due to the dextral movement of the Fa fault, forming 10 to 20 m wide structural breccia (Fig. 3a and c). Mineralization is mainly hosted in structural breccia and altered mafic tuff (Fig. 3a). Fault breccias, fault gouge, and fault cataclastic rocks are well developed within the fault zone, indicating brittle deformation (Fig. 3b; Yang et al., 2014a,b). The gentle strike change of Fa fault induces the bending of fault plane as well as change 3

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Fig. 3. Field photographs of the Suoluogou gold deposit. (a) Outcrop of orebody No. 15 controlled by Fa Fault and wall rocks. (b) Lamprophyre developed in Fa fault. (c) Slate breccia block in structural breccia. (d) Altered mafic tuff. (e) Carbonaceous slate. (f) Steep joint in mafic tuff. (g) Crosscutting relations of quartz veins, carbonate-quartz veins and carbonate-pyrite veins. (h) Stage Ⅳ pyrite veins crosscut carbonate-quartz veins. (i) Carbonate-pyrite veins of stage Ⅳ in altered mafic tuff. (j) Coarse-grained pyrite occur in the strong alteration area. Abbreviations: Cb = carbonate veins; Q + Cb = carbonate-quartz veins. 4

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Fig. 4. Backscattered electron (BSE) images and photomicrographs of mineralization assemblages in the Suoluogou deposit. (a) Pyrite of stage Ⅰ in carbonaceous slate. (b) Pyrite, chalcopyrite and magnetite in basalt. (c) Pyrite and arsenopyrite of stage Ⅱ in structural breccia. (d) Pyrite and arsenopyrite of stage Ⅱ in altered mafic tuff, showing a directed distribution. (e) The corerims texture of pyrite in structural breccia. (f) Pyrite and arsenopyrite of stage III in structural breccia. (g) The core-rim texture of pyrite in altered mafic tuff. (h) Carbonate-pyrite veins of stage Ⅳ. Abbreviations: Apy = arsenopyrite, Cb = carbonate, Ccp = chalcopyrite, Ger = gersdorffite, Mag = magnetite, Rt = rutile, Ser = sericite, Sp = sphalerite, Ttr = tetrahedrite.

3.2. Alteration and mineralization

of local stress in bends, which controlled the location of orebodies (Fig. 2c). The Fa fault was cut by a series of later NW-, SN-, and NEtrending faults (Fig. 2). There is no large scale igneous intrusion within the Suoluogou deposit, besides several dolerite and lamprophyre veins. The dolerite veins, mainly composed of plagioclase and augite, commonly intruded carbonaceous slate and mafic volcanic rock. Mineralization-related alterations, such as chloritization and sericitization (Fig. 5e), were observed in dolerite. Lamprophyre veins were generally emplaced along the Fa fault or cut through ore bodies (Figs. 2 and 3b). Phenocrysts in lamprophyre are mainly biotite with the matrix dominated by plagioclase and augite. Lamprophyre dykes have a biotite K-Ar age of 26.4–26.7 Ma (Zhang et al., 2015b), and mainly develop weak carbonation alteration, which is different from alteration associated with mineralization. This indicates the lamprophyre intrusion post-dated gold mineralization.

The deposit consists of eight orebodies, and the mineralization features can be best represented by the largest orebody No. 15. Gold ores were dominated by disseminated sulfide in alteration zone, and less significantly, by quartz-sulfide veins. Pyrite and arsenopyrite are the predominant sulfide mineral, with trace amounts of chalcopyrite, sphalerite, tetrahedrite, galena, and gersdorffite (Fig. 4). Rutile, sericite, apatite, and other trace minerals, such as barite, as well as the carbonaceous materials which were commonly observed in the carbonaceous slate, are included in, or coexist with pyrite (Figs. 4 and 5). Gold occurs as invisible gold in pyrite and arsenopyrite. The Au-carrying pyrite commonly occurs as disseminated grains, and less significantly, distributes along quartz veins or the shear foliation (Fig. 4c and d). Eeuhedral arsenopyrite is typically associated with pyrite. Outward from core of Fa, the degree of mineralization and the gold grade gradually decreased. Hydrothermal alteration is well-developed and primarily controlled 5

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Fig. 5. Microscopical and SEM photographs of the structural breccia (a and b), altered mafic tuff (c and d), dolerite (e), and carbonaceous slate (f, g, and h). Abbreviations: Cb = carbonate, Chl = chlorite, CM = carbonaceous material, Pl = plagioclase, Q + Cb = carbonate-quartz veins, Rt = rutile, Mag = magnetite, Brt = barite, Ser = sericite.

chloritization, which is common in the orogenic gold deposits related to shear zone (Roberts, 1987). Gold enrichment is closely related to the quartz-sericite-pyrite alteration assemblage.

by the Fa fault (Figs. 2 and 3a). The alteration involved a combination of silicification, carbonation, sericitization, chloritization, and sulfidation (Fig. 5). Silicification is widespread and occurs as quartz veins and stockworks, or aphanitic form. Sericitization is characterized by the presence of disseminated or massive sericite distributed in orebodies (Fig. 3a). Chloritization, generally distal to orebodies, is frequently associated with rutile (Fig. 5d). Carbonation represents the late stage of hydrothermal evolution, as indicated by carbonate veins crosscutting quartz veins and other alterations (Figs. 3g and 5a). From ore body to wallrock, the alteration gradually changed from sericitization to

3.3. Mineral paragenesis and mineralization stage According to crosscutting relations and mineral assemblages, four paragenetic stages can be divided in the Suoluogou gold deposit (Fig. 6). Stage Ⅰ is the pre-mineralization stage formed in the diagenetic process and magmatic crystallization, which is developed with pyrite 6

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sulfide stage (stage III). Stage Ⅱ is the main mineralization stage, represented by quartz-pyrite-arsenopyrite-sericite-chlorite assemblage. Pyrite occurs as euhedral, disseminated medium-grains, with overgrowth zone wrapping pre-existing crystallization-/diagenetic pyrite (Fig. 4d). Stage III with minor gold mineralization is represented by the carbonate mineral-quartz-sulfide veins, which cut the stage Ⅱ quartz vein (Figs. 3g and 5e). Minerals formed with this stage include pyrite, arsenopyrite, quartz, carbonate minerals, sericite with trace amounts of barite. Pyrite partly occurs along the carbonate mineral-quartz veins, and mainly occurs as euhedral and coarse grain with the overgrowth rim of early pyrite in structural breccia (Fig. 4f), and as subhedral to anhedral fine grains in altered mafic tuff (Fig. 4g). Stage Ⅳ is the post-mineralization stage characterized by carbonate mineral-pyrite veins, cutting the early veins of stage Ⅱ and III (Figs. 3g–i and 4h). 4. Methods 4.1. Sulfur stable isotopes Representative samples were collected along the section cross-cutting the ore body at different levels, containing ores, altered rocks and wall rock. Rock samples were cut and polished to make thin sections for microscopic observation and backscattered electron (BSE) scanning microscopy. Samples used for sulfur isotope analysis were selected from the specimens by microscopy to confirm that they could cover all stages of mineralization. The localities of those were shown in Fig. 7. Sulfur isotopes measured from 62 spots on pyrite from the Suoluogou ore are presented in Table 1. The backscattered electron (BSE) images of pyrite were prepared beforehand for in-situ sulfur isotopes determination. The in-situ sulfur isotope analysis of pyrite was carried out using the LA-MC-ICP-MS at the State Key Laboratory of Continental Dynamics, Northwest University. The system is comprised of a Resolution M50-LR excimer ArF laser ablation system coupled with a Nu Plasma 1700 MC-ICP-MS. The laser fluence was 3.6 J/cm2, and the frequency was 3 Hz, the spot size was 25–37 μm, the denudation model is single point denudation,

Fig. 6. Paragenetic sequence of the Suoluogou deposit. Abbreviations: Brt = barite, Apy = arsenopyrite, Cb = carbonate, Ccp = chalcopyrite, Chl = chlorite, CM = carbonaceous material, Ger = gersdorffite, Gn = galena, Mag = magnetite, Rt = rutile, Ser = sericite, Sp = sphalerite, Ttr = tetrahedrite, Ap = apatite.

and chalcopyrite (Fig. 4). The pyrite of this stage is wrapped in later hydrothermal pyrite in structural breccia and mafic volcanic rocks (Fig. 4e and g). Hydrothermal activities related to gold mineralization can be divided into quartz-sulfide stage (stage Ⅱ) and carbonate mineral-quartz-

Fig. 7. Geological section in the Suoluogou deposit, showing sulfur isotope data for pyrite. Among them, blue represent stage Ⅰ, red represent stage Ⅱ, green represent stage III, black represent stage Ⅳ. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.) 7

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Fig. 8. Backscattered electron (BSE) images showing δ34S values of pyrite. (a) and (b) Pyrite of stage Ⅰ in carbonaceous slate. (c) and (d) Pyrite of stage Ⅰ in mafic tuff. (e) Pyrite of stage Ⅰ in basalt. (f) and (g) Pyrite of stage Ⅰand stage Ⅱ in structural breccia, showing a core-rims texture. (h) Pyrite of stage Ⅰ, stage Ⅱ and stage III in structural breccia, showing a core-mantle-rims texture. Abbreviations: Apy = arsenopyrite, Cb = carbonate, Ccp = chalcopyrite, Ger = gersdorffite, Gn = galena, Mag = magnetite, Rt = rutile, Sp = sphalerite.

MC-ICP-MS method of solution injection. Standard samples used in the determination are IAEA-S-1, IAEA-S-2, and IAEA-S-3 (Ag2S powder). The δ34S values were calculated using the calibration method of standard-sample-bracketing (SSB). The 34S/32Sstandard is the mean isotope ratio of the two standard samples, which is measured once before and after the sample analysis. In order to monitor the accuracy of the data, a pair of laboratory internal standard samples will be tested every eight samples. Detailed instrumental conditions and analytical procedures are available in Chen et al. (2017), Bao et al. (2017) and Yuan et al. (2018).

the carrier gas was high purity He (280 mL/min), and the supplementary gas was Ar, generally 0.86 L/min. Mass spectrometer achieves > 20,000 resolution power by adjusting source slit, x-y slit, and adjustable collector slit in front of the Faraday cup. The sulfur isotope analysis generally uses a resolution power > 12,000. The data collection mode was TRA, with an integral time of 0.2 s, background collection time of 30 s, sample integral time of 50 s, and purge time of 75 s. The isotopic composition of sulfur is expressed as relative value: δxS = [(xS/32Ssample)/(xS/32Sstandard) − 1] * 1000; X is 34 or 33. The standard is the former international standard sample VCDT (Vienna Canyon Diablo Troilite), but the standard sample has been exhausted. Now, IAEA-S-1 (Ag2S, δ34S is known as −0.3‰) is used as the standard sample. All the laboratory standards for testing sulfur isotopes in this laboratory are determined by gas stable isotope mass spectrometry or

4.2. LA-ICP-MS mapping LA-ICP-MS mineral element mapping of pyrite was performed in the 8

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Fig. 9. Backscattered electron (BSE) images and photomicrographs showing δ34S values of pyrite. (a) Pyrite of stage Ⅰ and stage III in altered mafic tuff, showing a core-rims texture. (b) Pyrite of stage Ⅱ in altered mafic tuff. (c) and (d) Pyrite of stage Ⅱ in structural breccia. (e) and (f) Pyrite and arsenopyrite of stage III in structural breccia. (g) Pyrite and arsenopyrite of stage III in altered mafic tuff. (h) Pyrite veins of stage Ⅳ. Abbreviations: Apy = arsenopyrite, Cb = carbonate, Ccp = chalcopyrite, Rt = rutile.

5. Results

Ore Deposit and Exploration Centre (ODEC), School of Resources and Environmental Engineering, Hefei University of Technology, using a laser ablation system (PhotonMachines Analyte HE with 193-nm ArF Excimer), coupled to a quadrupole-based ICP-MS (Agilent 7900). Ablation was performed in an atmosphere of UHP He (0.9 L/min) mixed with Ar (0.9 L/min). Element maps were created by ablating sets of parallel line rasters in a grid across the sample. The laser beam was 10 mm, and the sample moved at a speed of 10 mm. The element mapping was performed at 10 Hz with energy of 2 J/cm2 after measuring the gas blank for 20 s. Standard sample NIST 610 were analyzed about 30 s for data calibration at the start and end of each mapping. Images were compiled and processed using the laboratory software LIMS (designed based on Matlab, Wang et al., 2017; Xiao et al., 2018) with 100% normalized calibration method.

In-situ analyses were performed on pyrite formed in various ore stages and hosted in different lithologies. To present the sulfur isotope distribution in different generations of growth zone, the sulfur isotopic values were systematically analyzed as shown in the BSE images and microscopic photos (Figs. 8 and 9). The δ34S values of stage Ⅰ range widely from −16.96‰ to 5.54‰, which largely depends on different lithology of host rocks (Fig. 10). The δ34S values of stage Ⅰ pyrite from the carbonaceous slate ranges from −14.9‰ to −16.96‰, from the basalt and the mafic tuff ranges from −6.63‰ to 5.54‰, and those from the structural breccia ranges from −4.45‰ to −10.23‰. In contrast, stage Ⅱ pyrite has a relatively narrow δ34S ranging from 6.01‰ to 8.59‰. The δ34S values for pyrite 9

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deposit (Kerrich and Wyman, 1990; Groves, 1993; Groves et al., 1998; Wang et al., 2019a, Li et al., 2019a,b). The Suoluogou orogenic gold deposits shows similarities to late Oligocene and Neogene Rotgulden orogenic gold deposits in the eastern Alps (Horner et al., 1997; Goldfarb et al., 2001). The deposits in Rotgulden, mined since pre-Roman times, were intimately related to the Tauern metamorphic dome during late orogenic extension (Horner et al., 1997). Greenschist facies alteration and brittle deformation conform to the classification of mesozonal orogenic gold deposits. The orebodies are mainly controlled by brecciated ores within shear zones, principally distributed at the bends of the structure (Horner et al., 1997). Arsenopyrite with pyrite and pyrrhotite in different proportions was the predominant mineral species in various deposits (Horner et al., 1997). 6.2. Sulfur isotope variation and its implication to fluid evolution In stage Ⅰ, the δ34S range of −6.63 to 5.54‰ of the pyrites from basalt, dolerite, and mafic tuff (Fig. 10) is consistent with the sulfur source of mafic volcanic rock, the δ34S of which is normally considered to be −5.7 to 7.6‰ (Fig. 12, Zhang and Gao, 2012). The δ34S range of −14.9 to −16.96‰ of the pyrites from the carbonaceous slate (Fig. 10) is a typical sulfur of reduction of seawater sulfate, indicating a synsedimentary origin (Chang et al., 2008; Zhao et al., 2018). The pyrites of stage Ⅰ from the structural breccia have δ34S values of −4.45 to −10.23‰ (Fig. 10), which can be explained by the mixing with hydrothermal as implied by the hydrothermal infiltration (Fig. 11). Ohmoto (1972) concluded that if the sulfur in the fluids is dominated by one species (e.g., H2S) and the relative isotopic enrichment factor between pyrite and the aqueous sulfur species is small. The mineral assemblage in the deposit is pyrite-arsenopyrite-chalcopyritesphalerite. Sulfate minerals are basically except trace amounts of barite presented in stage III, indicating that the sulfur in the initial ore fluid system is dominated by H2S (Zhang et al., 2013; Yang et al., 2016a,b). The δ34S value of pyrite can approximately reflect the sulfur isotope characteristic of ore fluid (Deng et al., 2015; Wang et al., 2015). The pyrite of the Suoluogou deposit have a decreasing δ34S signature through out the paragenetic sequence (Fig. 10, stage Ⅱ δ34S = 6.01 to 8.59‰, stage III δ34S = 0.96 to 4.62‰, stage Ⅳ δ34S = −11.12 to −16.11‰). Due to the complexity of fluid evolution, the measured sulfur isotope values may represent that the fluid could experience a fluid mixing and other processes, which modifies the fluid isotopes. Thus, in order to determine the ore fluid source, it is necessary to examine the fluid evolution of ore fluid. There are a variety of fluid evolution process that could result in a change of δ34S signature (Hodkiewicz et al., 2009; LaFlamme et al., 2018; Rye, 1993; Wang et al., 2018). In order to determine the most viable process, we carry out the detailed discussion below. The decreasing δ34S value of the fluid could be influenced by the mixture of magmatic-hydrothermal fluid (δ34S = 0 ± 5‰; Bowman, 1998). The magmatic rock developed in the mining area are dolerite and lamprophyre. The extensive ore-related hydrothermal alteration is observed in the dolerite (Fig. 5e), indicating that the dolerite is emplaced before mineralization. The lamprophyre dyke, with a biotite KAr age of 26.7–26.4 Ma (Zhang et al., 2015b) was cutting the ore body, was emplaced after mineralization. Therefore, the ore fluid could not be affected by magmatic-hydrothermal fluid. Wall rock reactions can influence the oxidation state and hence δ34S values of the ore fluid (Uemoto et al., 2002; Yang et al., 2018). Sulfidation of Fe oxides, and the reaction between reduced ore fluid and the pre-existing oxidised alteration assemblages (e.g. hematite or magnetite), could result in a significant change in the redox state of the hydrothermal fluids during gold mineralisation and thus negative shifts in δ34S of H2S (Phillips et al., 1986). But due to the absence of Fe oxides, oxidised alteration assemblages, and lack of reaction residues in the

Fig. 10. Histograms of δ34S values of pyrite in ore body and wall rocks in the Suoluogou deposit. From stage Ⅱ and stage Ⅳ, δ34S values gradually decreased.

from stage III show a lower distribution from 0.96‰ to 4.62‰. However, the δ34S values for pyrite from stage Ⅳ has a relatively negative value ranging from −11.12‰ to −16.11‰. Individual pyrite grain commonly consists of inner cores, middle mantles, and outmost overgrowth rims. The δ34S values of inner cores are similar to those of the stage Ⅰ pyrite, and the middle mantles and outmost overgrowth rims of pyrite grain correspond to the pyrite in stage Ⅱ and III, respectively (Fig. 8h). Multiple element maps of pyrites together with δ34S values from the different zones of pyrite from the Suoluogou deposits are shown in Fig. 11. The core (stage Ⅰ) has little gold and the δ34S values of −8.13‰ to −6.89‰. In the mantle (stage Ⅱ), the δ34S value is 8.05‰ where has a high content of gold. In the rim (stage III), the δ34S value is 3.34‰ and gold content is low. The main mineralization event was marked by the mantle zone with high As and Au, which is consistent with the geological observation that stage Ⅱ is the main mineralization stage. The hydrothermal pyrite are characterized by higher As and Au, and relatively lower Co, Ni, Sb, while the stage Ⅰ pyrite have relatively higher Co, Ni, Sb. As shown in LA-ICP-MS mapping (Au and As mapping in Fig. 11), the pyrite in the core has been obviously infiltrated by auriferous hydrothermal.

6. Discussion 6.1. Classification of genetic type of deposit and its analogue The Suoluogou gold deposit is located at the edge of crustal dome and is controlled by regional fault (Zhao et al., 2018). The deposit displayed disseminated and veinlet mineralization dominated by pyrite and arsenopyrite as gold-conveying minerals. Hydrothermal alteration comprises silicification, carbonation, sericitization, chloritization, and sulfidation. The presence of carbonate-chlorite alteration assemblages is consistent with the greenschist facies environment of the deposit (Groves, 1993). Mineralization, alteration, and structural control on mineralization all present typical features of mesozonal orogenic gold 10

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Fig. 11. LA-ICP-MS trace-element maps of pyrites from structural breccia. Three-zoned zones are shown in the Au and As maps, and Au is hosted in the middle zone. The BSE image shows the δ34S values of the different zones.

related pyrites (Nguyen, 1997; Yang et al., 2018). Rapid fluid pressure fluctuations can cause phase separation and/or continuous reactions with wall rocks by processes such as crack seal or hydraulic fracturing, resulting in the shifts in δ34S of ore fluid. As disscussed above, wall rock reactions and phase separation are not responsible for the negative shifts in δ34S of ore fluid. Furthermore, fluid pressure fluctuations commonly causes a larger variation in δ34S values and the wide range of δ34S values, which is also incongruent with the measured δ34S values of Suoluogou gold deposit (Hodkiewicz et al., 2009). The presence of trace amounts of barite supports the availability of isotope fractionation between oxidised and reduced sulfur species during the precipitation of oxidized minerals from ore fluids. Crossley et al. (2018) did calculations to assess the possible effect of isotope fractionation between oxidized and reduced sulfur species. The starting δ34S value composition was chosen as 8‰ for hydrothermal pyrite, which is the δ34S value of stage Ⅱ, representing the δ34S value of hydrothermal system. It was shown that a small amount of oxidised sulfur (SO2 and SO42−) leaving the fluid system can result in the decrease of several millesimal in isotope values. Due to the consumption of amounts of reduced sulfur with precipitation of pyrite in stage Ⅱ, the mole fraction of oxidized sulfur relative to the total sulfur (including oxidised and reduced sulfur species) could increase to be higher, resulting in the precipitation of barite from the ore fluids (Ohmoto, 1972; Hu et al., 2020). The precipitation amounts of barite could be small considering the low concentration of SO42− in ore fluids. Because of isotopic fractionation between oxidised and reduced sulfur species, the

orebody and wall rock, the above two reactions were ruled out. During wall rock carbonation, the reaction of CO2-bearing hydrothermal fluids with ferric minerals forms Fe-bearing carbonates, which would result in significant oxidation of the ore fluid (McCuaig and Kerrich, 1998; Palin and Xu 2000; Palin et al., 2001) and corresponding negative shifts in δ34S of H2S. Still the absence of ferric minerals and the presence of carbonaceous material, which indicates a reduced environment (Hu et al., 2016), negates that the role of carbonation. Phase separation is another avenue for oxidation of fluids, resulting in the negative shifts in δ34S (Rye, 1993). During phase separation, the ratio of SO4 to H2S in the residual ore fluid will increases due to the migration of reduced gases, such as H2S, from the liquid phase into the vapour phase (Drummond and Ohmoto, 1985). Under equilibrium conditions, this process leaves the residual ore fluid relatively oxidised and results in negative shifts in δ34S of precipitated sulfide minerals (Ohmoto, 1979; Ohmoto, 1986). But removal of H2S during phase separation also results in a rapid decrease in gold solubility, and furthermore results in gold deposition, which would be accompanied by increased hematite alteration (Mikucki and Groves, 1990; Cassidy et al., 1998). This is inconsistent with the small amount of gold deposited in stage III (Fig. 11) and the absence of hematite alteration in the deposit. Structures and fluid pressure fluctuations have potential influence on the δ34S value of ore-related pyrites (Hodkiewicz et al., 2009). During fault-valve cycles, large fluid pressure fluctuations establish different fluid-flow regimes, which influence physical and chemical conditions in the ore fluid, resulting in the change of δ34S values in ore11

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Fig. 12. “Box and whisker” plots of δ34S values of Suoluogou deposit, Ajialongwa deposit (Zhang et al., 2012), Gala deposit (Yan et al., 2013), Danba deposit and Yanzigou deposit (Zhao et al., 2018; Zhao, 2019). These are compared with variations in the sulfur isotopic compositions of sulfides in global sediment-hosted orogenic gold deposits through geologic time that relate to the time-dependant marine sulfate curve (Goldfarb et al., 1997; Chang et al., 2008; Zhao et al., 2018). Other δ34S values data: Orogenic gold deposit (Goldfarb and Groves, 2015); Metasomatism mantle wedge sulfide (Giuliani et al., 2016; Rielli et al., 2018); Enrichment mantle (Labidi et al., 2015); Mafic volcanic rock (Zhang and Gao, 2012); Mantle (Ohmoto, 1972); average oceanic crust and oceanic sediments (Rielli et al., 2018).

6.3. Crustal continuum model and source of ore fluids

precipitation of barite removes more heavy sulfur from the ore fluids relative to light sulfur, resulting in the decrease of sulfur isotope values of the residual fluids (Ohmoto, 1972). Therefore, fractionation between oxidised and reduced sulfur species in the open brecciated zone is explained to control the change of sulfur isotope values in the Suoluogou deposit. The decrease of δ34S value during mineral precipitation similar to that at the Suoluogou deposit, have been observed in many gold deposits around the world, such as Shanggong (Chen et al., 2008), Xincheng (Zhang et al., 2014), and Lady Bountiful (Cassidy and Bennett, 1993; Fig. 13). In the Eastern Goldfields Province of Yilgarn Craton, several Archean orogenic gold deposits have recorded the shifts in δ34S, including New Celebration (Hodge, 2010), Sunrise Dam (Brown et al., 2002), and Victory (Palin and Xu, 2000). Among them, Victory gold deposit, a world-class orogenic gold deposit, with a resource of approximately 250 t of gold, showed the negative shifts in δ34S, which has been described by Palin and Xu (2000). Mineralization of Victory occurs in hydrothermally altered slate and volcanic rock adjacent to shear zones and breccias (Palin and Xu, 2000). The distinct negative shifts in δ34S from ~3‰ to ~−4‰ has been interpreted as the result of progressive oxidation of ore fluid accompanying the mineralization (Palin and Xu, 2000).

Low concentrations of Au and As, detected by LA-ICP-MS, are found in the pyrites of stage Ⅰ (Fig. 11). In contrast, the pyrites of stage Ⅱ have high concentrations of Au and As, suggesting the pyrites during the crystallization-/diagenetic stage did not contribute enough Au to form ore. Au was likely introduced by a deep hydrothermal, which precipitated overgrowth on the preexisting pyrite (Liang et al., 2019). The gradual alteration centered around magmatic rock is absent in the deposit, indicating the ore fluid was not derived from the magmatic rock. In addition, the pyrites of stage Ⅳ have negative δ34S value (−11.12 to −16.11‰), which is consistent with the δ34S of carbonaceous slate (−14.9 to −16.96‰), indicating reactivation of sulfur in regional terrane. The pyrites of stage Ⅳ are gold-free, suggesting that the regional terrane have very limited capability to provide gold. As discussed above, the δ34S value of the stage Ⅱ (6.01 to 8.59‰) can best reflect the sulfur isotope of original ore fluid in the Suoluogou deposit, which falls within the normal range between about 0 and +10‰ for orogenic gold deposits (Fig. 12, Goldfarb and Groves, 2015). The comparison of δ34S values of Suoluogou and those from regional deposits could provide crucial clue for the fluid source. The δ34S value of sulfides in the primary gold deposits of the GLS are negative, such as Ajialongwa (δ34S = -8.91 to −12.02‰; Zhang et al., 2012) and Gala 12

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Fig. 13. Comparison diagram of sulfur isotope, host rock and gold grade between Suoluogou with Shanggong (Chen et al., 2008), Xincheng (Zhang et al., 2014), Lady Bountiful (Cassidy and Bennett, 1993), New Celebration (Hodge, 2010), Sunrise Dam (Brown et al., 2002), and Victory (Palin and Xu, 2000; Hodkiewicz et al., 2009).

(δ34S = -5.24 to −6.01‰; Fig. 12; Yan et al., 2013). In contrast, the δ34S value of sulfides in the hypozonal Danba and mesozonal Yanzigou, located in the northwestern margin of the Yangtze Craton, are 3.1 to 9.9‰, 8.5 to 10.7‰, respectively (Zhao et al., 2018; Zhao, 2019). The δ34S value of ore fluids at the Suoluogou deposit is in accordance with the δ34S value in the hypozonal and mesozonal gold deposit located in the northwestern margin of Yangtze Craton. The ore fluid of the hypozonal Danba gold deposit is approven to be formed by the devolatilization of the metasomatized lithospheric mantle, which is under the Neoproterozoic basement of the Yangtze Craton (Zhao et al., 2018; Zhao, 2019). Sulfur isotope values for mantle-derived fluid that deviate significantly from δ34S of 0‰ are commonly interpreted to reflect contributions of crust-derived S recycled into the Earth’s mantle via subduction (e.g., Giuliani et al., 2016; Alt and Shanks, 2006; Labidi et al., 2015). Zhou et al. (2002) proposed that the metasomatized lithospheric mantle was created by the southdipping subduction of oceanic crust, which was adjacent to the northwest margin of Yangtze Craton, in the Neoproterozoic (950–750 Ma). According to the crustal continuum model, the similar δ34S value indicates that the ore fluids of mesozonal Suoluogou and hypozonal Danba gold deposit could have similar sources, namely the metasomatized lithospheric mantle. This is consistent with the observation of Nie et al. (2018) about the Re-Os system of auriferous pyrite from Suoluogou deposit that the initial ratio of 187Os/188Os (0.178 ± 0.032) indicates a mantle source. Despite indeterminate, the comparison of sulfur isotope between the Suoluogou and global sediment-hosted orogenic gold deposits (Fig. 12) shows that Neoproterozoic crystalline basement or subduction-related sediment wedge are capable of providing sulfur for the pyrite of stage Ⅱ, which is similar to the Danba deposit. Zhou et al. (2002) reported that the basement of the Yidun island arc is similar to the basement of the northwestern margin of Yangtze Craton, which is widely considered to be the product of metamorphism of Neoproterozoic Panxi-Hannan arc assemblage (Zhao and Zhou, 2008). This support the opinion of that the source of ore fluid via devolatilization of the metasomatized mantle wedge above a subducting slab. The crustal continuum model, proposed based on the study of deposits with different depth characteristics in a number of discrete areas,

suggests that a majority of orogenic gold deposits are formed by a similar, but different evolutionary, ore fluid at various crustal depths (Groves, 1993; Groves et al., 1998). Due to the absence of single ore belt, in which gold deposits form a entire continuum (Groves, 1993), the mesozonal Suoluogou and the hypozonal Danba in the northwestern margin of the Yangtze Craton seem to constitute a rare case that the mesozonal and hypozonal orogenic gold deposits share a consistent source of ore fluid. 7. Conclusions The Suoluogou gold deposit is located in a poorly-documented gold province on the northwestern margin of the Yangtze Craton. A variety of research data from geology, ore mineralogy, in-situ sulfur isotopes, and LA-ICP-MS mapping of the pyrite demonstrate that Suoluogou is a typical mesozonal orogenic gold deposit. The wall-rock alteration, brittle deformation, and mineralization type present typical features of mesozonal deposit. The orebodies, hosted in the Late Triassic structural breccia and altered mafic tuff, are controlled by the bends of regional fault. Due to the absence of synchronous magmatic-hydrothermal fluid and the inconsistencies between our observations and other evolution processes, including fluid-rock interaction, phase separation, and fluidpressure fluctuations, the decreasing δ34S signature through out the paragenetic sequence is the result of the separation of oxidised sulfur species in the brecciated space. The precipitation of oxidised sulfur species result in the sulfur isotopic fractionations between oxidised and reduced sulfur species and the negative shifts in δ34S of ore fluid. The mesozonal Suoluogou orogenic gold deposit and the hypozonal Danba orogenic gold deposit were different levels of a crustal continuum model, in which the deposits share a consistent mantle source of ore fluid. Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. 13

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Acknowledgements

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