Pinaeva U, Ollier N, Cavani O, Balanzat E, Al-Sheikhly M, Wade T L, Clochard M-C
Laboratoire des Solides Irradiés CEA-CNRS-Ecole Polytechnique UMR7642, Institut Polytechnique de Paris, 91128, Palaiseau Cedex, France.
CIMAP, CEA-CNRS-ENSICAEN UMR6252, 14050, Caen Cedex, France.
Sci Rep. 2020 Apr 1;10(1):5776. doi: 10.1038/s41598-020-62792-4.
Sorption mechanism of uranyl by poly(bis[2-(methacryloyloxy)ethyl] phosphate) (PB2MP) functionalised polyvinylidene fluoride (PVDF) track-etched membranes, PB2MP-g-PVDF, was investigated. It was found that uranyl sorption obeyed Langmuir isotherm model giving a maximum U(VI) membrane uptake of 6.73 μmol g and an affinity constant of 9.85 ⋅ 10 L mol. XPS and TRPL measurements were performed to identify sorbed uranyl oxidation state and its environment. Uranyl was found to be mainly in its hexavalent state, i.e. U(VI), showing that the trapping inside the PB2MP-g-PVDF nanoporous membranes did not change the ion speciation. Two sorbed uranyl life-times (τ = 8.8 μs and τ = 102.8 μs) were measured by TRPL which pointed out different complexations taking place inside the nanopores. Uranyl sorption by PB2MP-g-PVDF membranes was also found to be pH dependent demonstrating the highest performance at circumneutral pH. In addition, TRPL was demonstrated to be not only a remarkable technique for U(VI) characterization, but also an alternative to voltammetry detection for trace on-site uranyl monitoring using PB2MP-g-PVDF nanoporous membranes.
研究了聚(双[2-(甲基丙烯酰氧基)乙基]磷酸酯)(PB2MP)功能化的聚偏氟乙烯(PVDF)径迹蚀刻膜PB2MP-g-PVDF对铀酰的吸附机制。发现铀酰吸附符合朗缪尔等温线模型,最大U(VI)膜吸附量为6.73 μmol g,亲和常数为9.85⋅10 L mol。进行了X射线光电子能谱(XPS)和时间分辨荧光光谱(TRPL)测量,以确定吸附的铀酰氧化态及其环境。发现铀酰主要处于六价态,即U(VI),这表明在PB2MP-g-PVDF纳米多孔膜内的捕获并没有改变离子形态。通过TRPL测量了两种吸附的铀酰寿命(τ = 8.8 μs和τ = 102.8 μs),这表明纳米孔内发生了不同的络合作用。还发现PB2MP-g-PVDF膜对铀酰的吸附依赖于pH值,在中性pH条件下表现出最高性能。此外,TRPL不仅被证明是一种用于U(VI)表征的卓越技术,而且是使用PB2MP-g-PVDF纳米多孔膜进行现场痕量铀酰监测的伏安法检测的替代方法。