Groundwater sulfate contamination in mining areas has attracted widespread attention. However, deciphering the source and evolution of sulfate in large-scale mining areas remains a challenge due to intense anthropogenic influences and complex hydrogeological conditions. In this study, 94 groundwater samples were analyzed by a combination of self-organizing maps, MixSiar model, multi-isotope analyses (δ34S, δ18OSO4, δD and δ18Owater) and hydrogeochemical methods to investigate the regional characteristics of groundwater sulfate source and evolution in China's largest coalfield (the Shenfuyu Coalfield). The results showed that the source and evolution of groundwater sulfate were controlled by human activities (mining and agricultural activities) and hydrogeological conditions. The groundwater sulfate primarily originated from pyrite oxidation, gypsum dissolution and human inputs. For the mining districts with shallow mining depths, pyrite oxidation and fertilizer contributed to groundwater sulfate. In addition, the ground cracks and abandoned mines controlled the BSR and pyrite oxidation processes. In contrast, the gypsum dissolution and cation exchange dominated the sulfate evolution in the mining districts with deep mining depths due to slow groundwater circulation. This study provided new insights into the source and evolution of groundwater sulfate in large coalfields, as well as references for regional water resource utilization and protection.
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