Rapid Sample Preparation for Alpha Spectroscopy with Ultrafiltration Membranes

Duval, Christine E.; Darge, Abenazer W.; Ruff, Cody; DeVol, Timothy A.; Husson, Scott M.

doi:10.1021/acs.analchem.8b00135

Cited by 20 publications

(14 citation statements)

References 18 publications

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“…Duval et al developed a method to graft EGMP from polyethersulfone membranes for the isotopic screening of waterborne uranium. After filtering solutions spiked with 233 U, the modified membranes achieved 233 U peak resolutions ranging from 17 to 33 keV FWHM [12]. Furthermore, the peak resolutions achieved by the membranes were sharp enough to distinguish 238 U (4.198 MeV) from 234 U (4.775 MeV) after filtering a spiked groundwater source at pH 6.…”

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confidence: 98%

Membranes for the Capture and Screening of Waterborne Plutonium Based on a Novel Pu-Extractive Copolymer Additive

2021

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This contribution describes the fabrication of plutonium-adsorptive membranes by non-solvent induced phase separation. The dope solution comprised poly(vinylidene fluoride) (PVDF) and a Pu-extractive copolymer additive of PVDF-g-poly(ethylene glycol methacrylate phosphate) (EGMP) in dimethylformamide (DMF). The effects of casting conditions on membrane permeability were determined for PVDF membranes prepared with 10 wt% PVDF-g-EGMP. Direct-flow filtration and alpha spectrometry showed that membranes containing the graft copolymer could recover Pu up to 59.9 ± 3.0% from deionized water and 19.3 ± 3.5% from synthetic seawater after filtering 10 mL of 0.5 Bq/mL 238Pu. SEM-EDS analysis indicated that the graft copolymer was distributed evenly throughout the entire depth of the copolymer membranes, likely attributing to the tailing observed in the alpha spectra for 238Pu. Despite the reduction in resolution, the membranes exhibited high Pu uptake at the conditions tested, and new membrane designs that promote copolymer surface migration are expected to improve alpha spectrometry peak energy resolutions. Findings from this study also can be used to guide the development of extractive membranes for chromatographic separation of actinides from contaminated groundwater sources.

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Section: Introductionmentioning

confidence: 98%

Membranes for the Capture and Screening of Waterborne Plutonium Based on a Novel Pu-Extractive Copolymer Additive

2021

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“…Beyond their use for separations, the sorbents can be integrated with sensing platforms. For example, membranes designed to bind uranium accelerated the preparation of samples for nuclear forensic analysis by alpha spectroscopy . Additionally, sorbents functionalized with terpyridine moieties captured heavy metal ions with high affinity (Figure C) and simultaneously served as fluorescent probes that quantified the extent of sorbent saturation …”

Section: Introductionmentioning

confidence: 99%

“…For example, membranes designed to bind uranium accelerated the preparation of samples for nuclear forensic analysis by alpha spectroscopy. 68 Additionally, sorbents functionalized with terpyridine moieties captured heavy metal ions with high affinity (Figure 1C) and simultaneously served as fluorescent probes that quantified the extent of sorbent saturation. 69 While the primary function of a membrane is to mediate transport, membrane reactors 70 that transform solutes as they permeate 71 can be realized by immobilizing catalysts along the pore walls.…”

Section: Introductionmentioning

confidence: 99%

100th Anniversary of Macromolecular Science Viewpoint: Integrated Membrane Systems

Hoffman

Phillip

2020

ACS Macro Lett.

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Membranes fabricated from self-assembled materials are one recent example of how polymer science has been leveraged to advance membrane technology. Due to their welldefined nanostructures, the performance of membranes made from these materials is pushing the boundaries of size-selective filtration. Still, there remains a need for higher performance and more selective membranes. The advent of functional membrane platforms that rely on mechanisms beyond steric hindrance (e.g., charge-selective membranes and membrane sorbents) is one approach to realize improved solute−solute selectivity and further advance membrane technology. To date, the lab-scale demonstration of these platforms has often relied on fabrication schemes that require extended processing times. However, in order to translate lab-scale demonstrations to larger-scale implementation, it is critical that the rate of the functionalization scheme is reconciled with membrane manufacturing rates. In this viewpoint, it is postulated that substrates lined by reactive moieties that are amenable to postfabrication modification would enable the production of membranes with controlled nanostructures while providing access to a diverse array of pore wall chemistries. A comparison of reaction and manufacturing rates suggests that mechanisms that exhibit second-order reaction rate constants of at least 1 M −1 s −1 are needed for roll-to-roll processing. Furthermore, for mechanisms that exhibit rate constants greater than 300 M −1 s −1 , it may be possible to integrate multiple functional domains over the membrane surface such that useful properties emerge. These multifunctional systems can expand the capabilities of membranes when the patterned chemistries interact at the heterojunctions between domains (e.g., Janus and charge-patterned mosaic membranes) or if they exhibit cooperative responses to external operating conditions (e.g., membrane pumps).

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“…In recent studies, functionalized polymer films and thin-film composite membranes have been demonstrated for the extraction and screening of various radioisotopes in water. − Combined with alpha spectrometry, these substrates greatly reduce the time involved for isotopic screening by combining purification, concentration, and sample mounting steps. Approaches to developing the functionalized polymer thin films fall into two general categories, the first being physical immobilization or encapsulation of extractive ligands into a polymer matrix, akin to how an extractive chromatography resin is formed.…”

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“…fwhm values for the alpha spectra of the Pu loaded on the grafted membranes were 28− 35 keV and were comparable to sources evaporated onto planchettes; however, significant tail contributions occurred in the grafted membranes due to Pu ions bound within the 1−1.5 μm thick samples. Duval et al 12 developed a UV-grafting method to modify PES ultrafiltration membranes with an extractive layer comprised of ethylene glycol methacrylate phosphate for capturing of uranium from groundwater. Using a 50 mL ultrafiltration cell, solutions spiked with 233 U were passed through the modified membranes, and the resulting uranium recoveries ranged from 81 to 88% for both deionized and simulated groundwater samples.…”

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Functionalized Polymer Thin Films for Plutonium Capture and Isotopic Screening from Aqueous Sources

et al. 2020

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The rapid screening of plutonium from aqueous sources remains a critical challenge for nuclear nonproliferation efforts. The determination of trace-level Pu isotopes in water requires offsite sample preparation and analysis; therefore, new methods that combine plutonium purification, concentration, and isotopic screening in a fieldable detection system will provide an invaluable tool for nuclear safeguards. This contribution describes the development and characterization of thin polymer–ligand films for the isolation and concentration of waterborne Pu for direct spectroscopic analyses. Submicron thin films were prepared through spin coating onto Si wafers and consisted of combinations of polystyrene (PS) with dibenzoylmethane, thenoyltrifluoroacetone, and di(2-ethylhexyl)phosphoric acid (HDEHP). Pu uptake studies from solutions at pH from 2.3 to 6.3 indicated that only films containing HDEHP exhibited significant recovery of Pu. High alpha spectroscopy peak energy resolutions were achieved for PS-HDEHP films over a range of film thicknesses from 30 to 250 nm. A separate study was performed to evaluate uptake from a primarily Pu(V) solution where it was observed that doubling the HDEHP loading in the film increased uptake of Pu by an order of magnitude. X-ray photoelectron spectroscopy (XPS) analysis revealed that HDEHP was highly concentrated within the first few nanometers of the film at the higher loading. XPS analysis also revealed that, in the presence of water, HDEHP was stripped from the surface layer of the film at circumneutral pH. While significant losses of ligand were seen in all samples, higher loadings of HDEHP resulted in measurable amounts of ligand retained after a 12-h soak in water. Findings of this study are being used to guide the development of thin-film composite membrane-based detection methods for the rapid, fieldable analysis of Pu in water.

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Rapid Sample Preparation for Alpha Spectroscopy with Ultrafiltration Membranes

Cited by 20 publications

References 18 publications

Membranes for the Capture and Screening of Waterborne Plutonium Based on a Novel Pu-Extractive Copolymer Additive

Membranes for the Capture and Screening of Waterborne Plutonium Based on a Novel Pu-Extractive Copolymer Additive

100th Anniversary of Macromolecular Science Viewpoint: Integrated Membrane Systems

Functionalized Polymer Thin Films for Plutonium Capture and Isotopic Screening from Aqueous Sources

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