Stratiform Cu-Co deposits hosted in (meta-) sedimentary and volcaniclastic rocks contribute two-thirds of the global Co supply. However, the mechanisms driving Co remobilization during tectonic-hydrothermal overprinting events remain poorly understood. As a dominant Co repository, pyrite can provide valuable insights into mineralization history due to its refractory nature. Here, we present the first micro-analytical investigation of pyrite from the Tuolugou Co(–Au) deposit in East Kunlun Orogenic Belt. Ore textures indicate that Co mineralization is attributed to two distinct stages: primary enrichment and subsequent overprinting processes. The former is characterized by pyrite (PyI with up to 3.92 wt% Co) remnants exhibiting oscillatory zones, while the latter is marked by deformation of pyrite (PyII) ores. Three overprinting episodes, namely Da, Db, and Dc, are further distinguished according to varying extents of deformation and mineral assemblages. The Da is characterized by synkinematic PyIIa (up to 4.18 wt% Co) augens, which were most likely formed via pressure–solution mechanism. The Db is represented by polygonal PyIIb (up to 4.75 wt% Co) and siegenite with 120° triple–point junctions. The random orientation and rare intragrain misorientation of cobaltiferous sulfides at Db suggest their formation by recrystallization without plastic strains. The Dc resulted in the formation of Co ± As–rich PyIIc (up to 5.36 wt% Co) along with minor occurrence of cobaltite–gersdorffite, pyrrhotite (up to 1.25 wt% Co), and marcasite (up to 1.28 wt% Co). The PyIIc replacing PyI underscores the role of fluid-coupled dissolution and precipitation during fluid–rock interactions in the formation of these cobaltiferous sulfide assemblages at Dc. The presence of PyIIc infilling within the PyI fissures, in conjunction with the transition from siegenite to cobaltite–gersdorffite, suggests a shift towards low fO2 and low temperature conditions under relatively brittle setting. There is a discernible disparity in sulfur isotope compositions between the two mineralization stages. The PyI exhibits a narrow range of δ34SV–CDT values from –2.14 to 1.35 ‰, indicating a magmatic sulfur origin. In contrast, PyII displays a wide δ34SV–CDT range of –5.22 to 6.16 ‰, suggesting an involvement of strata sulfur during the overprinting stage. Monazite U-Pb dating has effectively constrained two mineralization events. The ca. 453 Ma age implies a potential correlation of the primary Co mineralization with the Late Ordovician to Early Silurian exhalative-syngenetic processes in a Proto–Tethyan-related post–collisional extension setting. Conversely, the ca. 190 Ma age indicates that Co remobilization was instigated by the early Mesozoic ductile–brittle deformation associated with the Paleo-Tethyan orogenesis. Finally, geochemical modeling was performed by simulating the interaction of a Co-rich acidic, reducing fluid with typical quartz-albitite rocks. The simulations demonstrate the appearance of independent Co minerals such as Co-pentlandite during the reaction progression, greatly supporting ore upgrading via tectonic-hydrothermal overprinting.
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