Separation of Radioactive Ruthenium from Alkaline Solution: A Solvent Extraction and Detailed Mechanistic Approach

Abstract

A solvent extraction-based technique has been utilized to study the separation of ruthenium from simulated alkaline solution using Aliquat 336 as the extractant and isodecyl alcohol (IDA) as the phase modifier in n-dodecane. The effects of various experimental parameters such as solution pH, mixing time, concentration of Aliquat 336 and IDA, role of citric acid as the aqueous phase modifier/complexing agent, and stripping agents have been evaluated. It was observed that with the increase in the solution pH, the extraction efficiency increases gradually. However, when citric acid was added into the aqueous solution, an overall increase (from ∼20 to 91%) in ruthenium extraction is observed. 20 min of the mixing time was found to be sufficient to reach the extraction equilibrium. Solution composition was optimized as 50% Aliquat 336 and 10% IDA in n-dodecane (v/v) for maximum extraction. The stripping of ruthenium from the loaded organic phase has been studied using HCl and HNO3. The result indicates that in the presence of 8 M HNO3, ∼73% of ruthenium can be back extracted to the aqueous phase in a single contact. The stripping efficiency of HNO3 was found to be higher than that of HCl. Active studies with 106Ru as the radiotracer were also performed and monitored using a HPGe detector. The same method was implemented for extraction studies with real waste solution in the presence of other radionuclides such as 137Cs, 90Sr, and 125Sb. The presence of the chemical species in aqueous as well as organic phase has been identified using UV–vis spectrophotometry, Fourier transform infrared spectroscopy, and Raman spectroscopy. Density functional theory-based quantum mechanical calculations have been performed in order to unravel the extraction mechanism with the present solvent system.