Distribution of uranium in soil components of agricultural fields after long-term application of phosphate fertilizers

Long-term application of phosphate fertilizers causes accumulation of U in the surface soil of agricultural fields. We investigated the soil constituents that contribute to the accumulation of U by using chemical extraction methods. Surface soil samples were obtained from upland fields, pastures, and paddy fields cultivated without any phosphate fertilizer (control site), with NPK fertilizer (NPK site), and with both NPK fertilizer and compost (NPK+compost site) for more than 20 years. In addition to the total U (Ut) concentration in soil, the concentrations of pyrophosphate- and acid oxalate-extractable U were determined as a measure of U associated with soil organic matter and poorly crystalline Fe/Al minerals in soil, respectively. The total, pyrophosphate-extractable, and acid oxalate-extractable U concentrations were higher in the soil obtained from the NPK and NPK+compost sites than in that obtained from the control site. The difference in the U concentrations between the NPK or NPK+compost site and the control site corresponded with the increased U concentration observed after the application of the phosphate fertilizer or both the fertilizer and compost. In the upland field and pasture soil, the increase in pyrophosphate-extractable U was 83-94% of that in Ut. On the other hand, the increase in acid oxalate-extractable U was 44-58% of that in Ut in the upland field and pasture soil, but it was almost equivalent to the increase in Ut in the paddy soil with NPK. In conclusion, most of the phosphate fertilizer-derived U was either incorporated into the soil organic matter or poorly crystalline Fe/Al minerals in the surface soil of agricultural fields. Thus, soil organic matter is an important pool of U in upland field and pasture soil, whereas poorly crystalline Fe/Al minerals are important pools of U in paddy soil experiencing alternating changes in redox conditions.