Chemical Composition of Hydrothermal Pyrite as an Indicator for Deciphering Ore-Forming Processes: A Case Study from the Mamuniyeh Copper Deposit, UDMA

زمین شناسی اقتصادی

Articles in Press, Accepted Manuscript, Available Online from 17 March 2025   

Document Type: Research Article

DOI: 10.22067/econg.2025.1131

Authors

Mohammad Goudarzi^{* 1}; Hassan Zamanian²; Urs Klötzli³; Matee Ullah⁴

¹Ph.D., Department of Geology, Faculty of Basic Science, Lorestan University, Khorramabad, Iran

²Professor, Department of Geology, Faculty of Science, University of Tehran, Tehran, Iran

³Professor, Department of Lithospheric Research, Faculty of Earth Sciences, Geography and Astronomy, University of Vienna, Vienna, Austria

⁴Ph.D., Department of Lithospheric Research, Faculty of Earth Sciences, Geography and Astronomy, University of Vienna, Vienna, Austria

Abstract

The major and trace element content in hydrothermal pyrite was analyzed, as the most abundant sulfide mineral associated with quartz veins, to reveal ore-forming processes in the Mamuniyeh deposite, central Urumieh-Dokhtar Magmatic Arc. The Co–Ni–As signatures in pyrite is closely linked to the genetic model and geological processes of the deposits. Cobalt, nickel, and arsenic data from the Mamuniyeh pyrites indicate a predominance towards the cobalt region, consistent with hydrothermal and epithermal magmatic ore deposits. Data shows fluid evolution from primary magmatic water to later meteoric waters, with magmatic water dominating the early stages and meteoric waters added later. The reduction in arsenic content in pyrites, due to the mixing of the ore-forming fluid with oxygen-rich meteoric waters, leads to an increase in arsenic concentration in the system. Under oxidizing conditions, arsenic with an oxidation state of As¹⁻ substitutes for sulfur, and in combination with Fe²⁺, it incorporates into the pyrite structure as As³⁺ and As⁵⁺. Vertical zoning of elements in epithermal systems suggests that most Mamuniyeh samples exhibit characteristics of the middle part of the mineralization system and somewhat deeper zones. Copper contents in the Mamuniyeh pyrites, up to 1.1 wt.%, indicate pyrite can act as a significant copper absorber. Nickel contents in the Mamuniyeh pyrites (up to 0.34 wt.%) are higher than continental crust nickel, indicating a mantle origin of them. Variations in Ni/Co ratios in pyrite for classifying hydrothermal deposit origins show a dominant range between 1 and 10, consistent with magmatic-hydrothermal origin, likely formed by fluid-rock interactions between magmatic-hydrothermal fluids and volcanic host rocks.
 
Introduction
Pyrite as the most common sulfide mineral in the Earth's crust, widely exists in magmatic-hydrothermal systems (Reich et al., 2013; Deditius et al., 2014; Dubosq et al., 2018). The rare element content in pyrite can reflect the conditions of the mineralizing fluid, such as temperature, pH, and oxygen fugacity, as well as the mechanisms of element formation and deposition during fluid evolution and ore formation (Agangi et al., 2014; Sykora et al., 2018). Pyrite commonly plays a vital role in determining the distribution of rare elements and heavy metals in these systems and can effectively control the distribution of economically valuable elements such as silver, arsenic, gold, and heavy metals (Large et al., 2009; Cook et al., 2013; Agangi et al., 2014). Given pyrite's ubiquity and its capacity to host many rare elements (e.g., Co, Ni, Cu, As, Se, Ag, Sb, Te, Pb, Bi, and Au), its chemistry has been successfully used to trace the physicochemical evolution of hydrothermal fluids and to reveal formation processes in various mineral deposits (e.g., Carlin-type gold, Cline, 2001; Large et al., 2009; epithermal gold, Deditius et al., 2008; Kouhestani et al., 2017; orogenic gold, Wu et al., 2019; volcanogenic massive sulfide, Martin et al., 2022; porphyry copper (gold), Reich et al., 2013, Keith et al., 2022). The aim of this studyis to analyze chemistry of pyrite in the low-sulfidation epithermal copper mineralization system in southern Mamuniyeh. The findings will enhance the understanding of the epithermal mineralization processes and magmatic evolution in this region. The results provide insights into the fluid evolution and ore formation processes within the epithermal system, contributing to a broader understanding of mineral deposit formation.
 
Geology and Petrography
Mamuniyeh epithermal system includes significant rock outcrops composed of intrusive rocks such as gabbro, diorite, and monzodiorite, along with a series of acidic to basic volcanic rocks. These include andesite tuff, pyroxene andesite-andesite porphyry, dacite-rhyodacite tuff, acidic lava, basaltic andesite, diabase, and basalt-diabase (Goudarzi et al., 2024a). According to the 1:100,000 scale geological map of Zaviyeh (Amidi et al., 2004), the volcanic and pyroclastic units are of Eocene age, while the intrusive units likely intruded during the Oligocene to Early Miocene periods. Geochemical characteristics show that these magmatic series are calc-alkaline, significantly influenced by mantle metasomatism (Rezaei Kahkhaei et al., 2014). Features like LILE enrichment over HFSE, negative Nb and Ti anomalies, and highly positive lead anomalies indicate calc-alkaline magmatism associated with a subduction zone, with crustal contamination during the ascent of the parent magma in this region (Goudarzi et al., 2024a).
 
Mineralization and Mineralography
The main copper mineralization in the Mamuniyeh epithermal system features veins and veinlets aligned with regional structures. Primary mineralization includes quartz with sulfide minerals like chalcopyrite, pyrite, and bornite, and oxide minerals such as specularite. Pyrite, the most abundant sulfide, appears in two generations. The first generation consists of framboidal and semi-euhedral pyrite, which can be fine- to coarse-grained and sometimes altered to hematite and goethite (Goudarzi et al., 2024c). The second-generation forms vein and veinlet fillings and occasionally include inclusions within chalcopyrite. Pyrite occurs in various assemblages: quartz + pyrite (Qz+Py); quartz + chalcopyrite + pyrite (Qz+Ccp+Py); quartz + specular hematite + pyrite (Qz+Py+Hem); and quartz + chalcopyrite + specular hematite ± pyrite ± bornite (Qz+Ccp+Hem±Py±Bn), found in replacement, breccia, disseminated, and colloform textures.
 
Vein/Veinlet Pyrite

Quartz + Pyrite (Qz+Py): Oldest veins, 1-20 mm thick, with coarse, euhedral pyrite grains
Quartz + Chalcopyrite + Pyrite (Qz+Ccp+Py): Veins contain chalcopyrite (50%), pyrite (30%), and quartz (20%), 1 mm to 5 cm thick
Quartz + Chalcopyrite + Specular Hematite ± Pyrite ± Bornite (Qz+Ccp+Hem±Py±Bor): Most common, 0.5-5 cm thick, with chalcopyrite (40%), specular hematite (30%), pyrite (10%), bornite (5%), and quartz (15%)
Quartz + Specular Hematite + Pyrite (Qz+Py+Hem): Veins, 0.5-10 cm thick, contain specular hematite (60%), pyrite (10%), and quartz (20%)

 
Other types of Pyrite mineralization

Disseminated type: Euhedral to anhedral pyrite crystals spread within intrusive and volcanic rocks and quartz veins
Colloform type: Rapid, low-temperature quartz deposition in shallow epithermal systems, forming alternating ore-bearing and ore-free bands
Crustiform type: Periodic temperature fluctuations and fluid changes during boiling, forming colloform banding with iron oxides, hematite, pyrite, and secondary copper minerals
Hydrothermal Breccia Mineralization: Hydraulic fracturing from fluid pressure increases, creating breccia with ore mineral fragments like pyrite, indicative of boiling processes

 
Research Methodology
After thorough field examinations of surface outcrops and drill cores, 70 polished sections from mineralized zones and veins containing sulfide and oxide minerals were collected for ore and mineralogical studies. Suitable sulfide samples from 8 polished sections were re-examined using an electron microscope and BSE images. Following carbon coating, the samples were analysed using a CAMECA SX Five Electron Microprobe equipped with a field emission cathode and energy-dispersive X-ray (EDX) system. This setup, with a 20 kV accelerating potential, 25 nA probe current, and 60 µm beam diameter, enabled rapid semi-quantitative elemental analysis in the Department of Lithospheric Research laboratory at the University of Vienna.
 
Results and Discussion
EPMA analysis on 58 points in pyrite shows no gold presence and very low silver concentration, up to 0.05 wt.%. Maximum concentrations of elements measured are arsenic (0.20 wt.%), lead (0.26 wt.%), copper (0.95 wt.%), antimony (0.23 wt.%), tin (0.04 wt.%), zinc (0.018 wt.%), nickel (0.34 wt.%), and cobalt (1.12 wt.%). Strong element correlations in pyrite include tin with zinc, arsenic with lead, manganese with zinc, and manganese with silver. BSE images show pyrite in oxide-sulfide veins as individual grains, often with chalcopyrite at the edges or as inclusions within chalcopyrite. Element variation diagrams for the Mamuniyeh pyrites indicate no significant changes in iron and sulfur with increasing arsenic. Cobalt content increases, while copper decreases with more iron. Cobalt and nickel show a stable relationship. Copper increases with zinc, while silver decreases with increasing arsenic and antimony but increases with tin. Previous studies indicate that the composition of trace elements in sulfides is controlled by the physicochemical conditions of hydrothermal fluids, such as temperature, pH, and redox conditions, revealing ore-forming processes in hydrothermal environments (Reich et al., 2013; Large et al., 2014; Gregory et al., 2016; Sykora et al., 2018; Saravanan Chinnasamy et al., 2021). For example, Te content in pyrite is mainly influenced by oxygen fugacity and pH, whereas As and Se are likely controlled by temperature (Huston et al., 1995; Deditius et al., 2008; Keith et al., 2018). The Co–Ni–As ratio in pyrite correlates closely with the deposit's genetic model and geological processes (Loftus-Hills and Solomon, 1967; Yan et al., 2012). Co, Ni, and As data plots for the Mamuniyeh pyrites indicate samples skewed towards the cobalt region, typical of magmatic-hydrothermal and epithermal deposits (Yan et al., 2012; Niu et al., 2016) (Fig. 7A). S-As substitution degree in pyrite is a temperature indicator, showing arsenic enrichment at lower temperatures (Kusebauch et al., 2018). Co and Ni are mantle-derived elements; Ni is usually concentrated in early-stage magmatic minerals, decreasing gradually with magmatic evolution, while Co increases (Kusebauch et al., 2018; Niu et al., 2016). Arsenic content depends on meteoric and magmatic water ratios, with higher arsenic content indicating a meteoric water role. If magmatic water predominates, samples plot towards Co; with meteoric water dominance, samples plot closer to arsenic (Yan et al., 2012). The plotted data suggests fluid evolution from initial magmatic water to later meteoric water. Reduction of arsenic content in pyrites, due to the mixing of hydrothermal vein fluid with high-oxygen-fugacity meteoric water, may increase arsenic content. Under oxidizing conditions, arsenic content decreases as arsenic replaces S in the pyrite structure (Cook and Chryssoulis, 1990; Liang et al., 2013). Geochemical studies have shown vertical zoning in epithermal systems (Boyle, 1979), with As, Sb, Hg, Ba, and Ag dominant in the upper parts; Cu, Pb, Zn, and Bi in the middle parts; and Co, Ni, Ti, and Cr in deeper parts. Mamuniyeh's system mainly shows middle to deep characteristics. Studies indicate that copper can significantly incorporate into pyrite's structure, sometimes reaching notable weight percentages (Einaudi, 1968; Clark, 1970; Pacevski et al., 2008). In Mamuniyeh, copper concentrations in pyrite reach up to 1.1 wt.%, showing pyrite as a substantial copper host. Due to large ionic size, lead rarely enters pyrite's lattice and typically deposits as galena (Huerta-Diaz and Morse, 1992; Koglin et al., 2010). Pyrite can also trap elements like silver, antimony, and tin when remobilized, though their contents in the Mamuniyeh pyrites are minimal (0.05 wt.%, 0.02 wt.%, and 0.002 wt.%, respectively). Nickel, easily incorporated into pyrite, remains even during recrystallization (Huerta-Diaz and Morse, 1992). High nickel content in the Mamuniyeh pyrites (0.34 wt.%) suggests a mafic-ultramafic mantle source (Palme and O'Neill, 2003; Zhao et al., 2011), exceeding continental crust levels (Rudnick and Gao, 2014). Nickel’s solubility limit is around 10 mol% NiS₂ in pyrite while cobalt can fully mix into pyrite at temperatures above 700 °C (Abraitis et al., 2004), making Co concentration in pyrite a useful geothermometer (Zhao et al., 2011). Co/Ni ratios in pyrite, unaffected by slight differences in Co and Ni affinities for chloride ligands, reflect hydrothermal deposit conditions (Bralia et al., 1979; Bajwah et al., 1987). In Mamuniyeh, Co/Ni ratios between 1 and 10 indicate a magmatic-hydrothermal origin (Reich et al., 2016), consistent with previously defined characteristics.
 
 

Keywords

Pyrite Chemistry; Epithermal; Low Sulfidation; Copper; EPMA; Trace Elements; Urumieh-Dokhtar Magmatic Arc (UDMA)

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