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The oxidative alteration of uraninite and the fate of trace elements (Y, LREE, Zr, and Th) in a granite-hosted uranium ore deposit in north Guangdong province, China, were investigated to understand the geochemical behavior of spent UO 2  fuel and associated fission products and transuranium elements under oxidizing conditions. In light of the paragenetic relationship of the alteration products, two alteration series of uraninite were identified: one is the silicate series with a mineral paragenesis of uraninite → uranyl oxide hydrates → Si-rich uranyl phase → uranophane (Ca[(UO 2 )(SiO 3 OH)] 2 (H 2 O) 5 ), and the other is the phosphate series with a mineral paragenesis of uraninite → uranyl oxide hydrates → autunite (Ca[(UO 2 )(PO 4 )] 2 (H 2 O) 6 ) → yingjiangite ((K 2 ,Ca)(UO 2 ) 7 (PO 4 ) 4 (OH) 6 (H 2 O) 6 ). In contrast to the wide distribution and abundance of uranophane and the uranyl phosphate minerals, uranyl oxides were only occasionally found in the ore samples, suggesting that the uranyl silicates and phosphates should be the predominant alteration products of UO 2  under oxidizing conditions, although uranyl oxide hydrates would be the solubility-limiting phase of uranium in the very early stage of alteration. Furthermore, the interlayer cation of the uranyl phases in the Xiazhuang uranium ore field is dominated by Ca 2+ , indicating that the release of uranium and other radionuclides will be limited mainly by uranophane and autunite during the oxidative alteration of spent UO 2  fuel in underground repositories where enhanced calcium concentration is expected due to cement/water reactions.

Trace element immobilization by uranyl minerals in granite-hosted uranium ores: Evidences from the Xiazhuang ore field of Guangdong province, China