The recently discovered Sanjiu ore field (SJOF) is a granite-related uranium ore field located in the middle of Zhuguangshan (South China). The relationship between hydrothermal alteration of granite and uranium mineralization in the SJOF is crucial yet understudied. In this study, the major- and trace-element contents of granite samples (fresh granite, altered granite, and tectonites) with different uranium contents were analyzed by using X-ray fluorescence spectroscopy (XRF) and inductively coupled plasma–mass spectrometry (ICP–MS). The analytical results show a relative increase in Si, S, Ca, Pb, Mo, and Sb content in altered granites and tectonites, relative to fresh granites. During the mineralization stage, the increase of the aforementioned elements is related to various hydrothermal alterations (e.g., silicification, carbonation, sulfation, etc.) and newly formed minerals (e.g., microfine crystalline quartz veins; calcite agglomerates or fine veins; and metal sulfides, such as pyrite). There is a concomitant relative decrease in Na, K, Al, Fe, Mg, and other elemental contents that may be due to mineralogical alteration processes, such as biotite to chlorite, feldspar-group minerals to clay minerals, and redox of Fe-bearing minerals. The LREE/HREE ratio in altered granites decreases significantly with the increase in uranium content, suggesting that a low LREE/HREE ratio may be a prospecting indicator. The normalized trace-element patterns of mineralized granite (ore) and the relatively high U content of fresh granite imply that granitic rocks may be the primary uranium source in the SJOF. The uranium mineralization is mainly concentrated in the redox zone that occurs at a depth of 100−300 m. The redox zone is characterized by the most developed hydrothermal alterations and enrichment of trace elements, including W, Mo, Sb, Li, and the HREE.
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