Polyamidoxime-based membranes for the rapid screening of uranium isotopes in water.

Traditional radiochemistry approaches for the detection of trace-level alpha-emitting radioisotopes in water require lengthy offsite sample preparations and do not lend themselves to rapid quantification. Therefore, a novel platform is needed that combines onsite purification, concentration, and isotopic screening with a fieldable detection system. This contribution describes the synthesis and characterization of polyamidoxime membranes for isolation and concentration of uranium from aqueous matrices, including high-salinity seawater. The aim was to develop a field portable screening method for the rapid quantification of isotopic distribution by alpha spectroscopy. Membranes with varying degree of modification were prepared by chemical conversion of nitrile groups to amidoxime groups on the surface of polyacrylonitrile ultrafiltration (UFPAN) membranes. Attenuated total reflectance Fourier-transform infrared spectroscopy was used to analyze changes in surface chemistry. Flow through filtration experiments conducted using deionized (DI) water and simulated seawater solutions indicated that the modified membrane was effective in capturing more than 95% of the uranium in the solution prior to breakthrough even in the presence of salt ions. Batch uptake experiments were conducted and compared with the flow through experimental data to elucidate likely binding mechanisms. Alpha spectra of uranium loaded membranes were analyzed, and the effects of solution matrix and degree of modification on peak energy resolution were studied. Peak energy resolutions of 24 ± 2 keV and 32 ± 6 keV full width at half maximum (FWHM) were obtained by loading uranium from DI and seawater solutions onto modified membranes. Full width at 10% maximum of the same spectra were calculated to be 63 ± 9 keV and 160 ± 34 keV to quantify differences seen in peak tailing. Calculations performed based on the results show that it would take less than 3 h of analysis time to screen a sample provided enough volumes of solution are available. This work offers a facile method to prepare polyamidoxime-based membranes for uranium separation and concentration at circumneutral pH values, enabling the rapid, onsite screening of unknown samples.

Rapid Sample Preparation for Alpha Spectroscopy with Ultrafiltration Membranes.

This contribution describes a rapid, fieldable alpha spectroscopy sample preparation technique that minimizes consumables and decreases the nuclear forensics timeline. Functional ultrafiltration membranes are presented that selectively concentrate uranium directly from pH 6 groundwater and serve as the alpha spectroscopy substrate. Membranes were prepared by ultraviolet grafting of uranium-selective polymer chains from the membrane surface. Membranes were characterized by Fourier-transform infrared spectroscopy before and after modification to support functionalization. Membrane performance was evaluated using uranium-233 or depleted uranium in both deionized and simulated groundwater at pH 6. Functionalized membranes achieved peak energy resolutions of 31 ± 2 keV and recoveries of 81 ± 4% when prepared directly from pH 6 simulated groundwater. For simulated groundwater spiked with depleted uranium, baseline energy resolution was achieved for both isotopes (uranium-238 and uranium-234). The porous, uranium-selective substrate designs can process liters per hour of uranium-contaminated groundwater using low-pressure (<150 kPa) filtration and a 45 mm diameter membrane filter, leading to a high-throughput, one-step concentration, purification, and sample mounting process.