Radionuclides,trace elements,and radium residence in phosphogypsum of Jordan

Voluminous stockpiles of phosphogypsum (PG) generated during the wet process production of phosphoric acid are stored at many sites around the world and pose problems for their safe storage, disposal, or utilization. A major concern is the elevated concentration of long-lived ²²⁶Ra (half-life = 1,600 years) inherited from the processed phosphate rock. Knowledge of the abundance and mode-of-occurrence of radium (Ra) in PG is critical for accurate prediction of Ra leachability and radon (Rn) emanation, and for prediction of radiation-exposure pathways to workers and to the public. The mean (±SD) of ²²⁶Ra concentrations in ten samples of Jordan PG is 601 ± 98 Bq/kg, which falls near the midrange of values reported for PG samples collected worldwide. Jordan PG generally shows no analytically significant enrichment (<10%) of ²²⁶Ra in the finer (<53 μm) grain size fraction. Phosphogypsum samples collected from two industrial sites with different sources of phosphate rock feedstock show consistent differences in concentration of ²²⁶Ra and rare earth elements, and also consistent trends of enrichment in these elements with increasing age of PG. Water-insoluble residues from Jordan PG constitute <10% of PG mass but contain 30–65% of the ²²⁶Ra. ²²⁶Ra correlates closely with Ba in the water-insoluble residues. Uniformly tiny (<10 μm) grains of barite (barium sulfate) observed with scanning electron microscopy have crystal morphologies that indicate their formation during the wet process. Barite is a well-documented and efficient scavenger of Ra from solution and is also very insoluble in water and mineral acids. Radium-bearing barite in PG influences the environmental mobility of radium and the radiation-exposure pathways near PG stockpiles.