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用激光荧光光谱法对羟硅钾铀矿[K(UO₂)(SiO₃OH)(H₂O)₁.₅]和水羟钾铀矿K₂[(UO₂)₃O₂(OH)₃]·2.7H₂O进行了表征。

Boltwoodite [K(UO2)(SiO3OH)(H2O)1.5] and compreignacite K2[(UO2)3O2(OH)3]2.7H2O characterized by laser fluorescence spectroscopy.

作者信息

Arnold Thuro, Baumann Nils

机构信息

FZ Dresden-Rossendorf, Institute of Radiochemistry, Dresden, Germany.

出版信息

Spectrochim Acta A Mol Biomol Spectrosc. 2009 Jan;71(5):1964-8. doi: 10.1016/j.saa.2008.07.029. Epub 2008 Jul 31.

Abstract

Synthetically prepared boltwoodite and compreignacite were characterized with time-resolved laser-induced fluorescence spectroscopy (TRLFS). The obtained TRLFS emission spectra of both synthesized uranium minerals differ from each other in their positions of the vibronic peak maxima and in their fluorescence lifetimes. Also, the shapes of the spectra and their respective intensities are different. The TRLFS-spectrum of boltwoodite showed well-resolved sharp vibronic peaks at 485.1, 501.5, 521.2, 543.0, 567.4, and 591.4nm with deep notches between them and compreignacite is characterized by two broad peaks with various shoulders. Here five emission bands were identified at 500.7, 516.1, 532.4, 554.3, and 579.6nm. The shape of the TRLFS spectra of compreignacite is typical for uranium in a hydroxide coordination environment. For both minerals two fluorescence lifetimes were extracted. The two species of boltwoodite and compreignacite, respectively, showed the same positions of the peak maxima showing that the coordination environments are similar, but differ in the chemistry and number of possible quenchers, e.g. water molecules and hydroxide groups. For boltwoodite fluorescence lifetimes of 382 and 2130ns, and for compreignacite shorter ones of 202 and 914ns, respectively, were determined. The spectroscopic signatures of the two uranyl minerals reported here could be useful for identifying uranyl(VI) mineral species as colloids, as thin coatings on minerals, as minor component in soils, or as alteration products of nuclear waste.

摘要

采用时间分辨激光诱导荧光光谱法(TRLFS)对合成的板铅铀矿和水碳铀矿进行了表征。两种合成铀矿物的TRLFS发射光谱在振动峰最大值位置和荧光寿命方面彼此不同。此外,光谱的形状及其各自的强度也不同。板铅铀矿的TRLFS光谱在485.1、501.5、521.2、543.0、567.4和591.4nm处显示出分辨率良好的尖锐振动峰,其间有深凹槽,而水碳铀矿的特征是有两个带有各种肩部的宽峰。在此,在500.7、516.1、532.4、554.3和579.6nm处识别出五个发射带。水碳铀矿的TRLFS光谱形状是铀在氢氧化物配位环境中的典型形状。对于这两种矿物,提取了两个荧光寿命。板铅铀矿和水碳铀矿这两种矿物分别在峰最大值位置相同,表明配位环境相似,但在化学性质和可能的猝灭剂数量(例如水分子和羟基)方面有所不同。板铅铀矿的荧光寿命分别为382和2130ns,水碳铀矿较短,分别为202和914ns。本文报道的两种铀酰矿物的光谱特征可用于识别作为胶体、矿物上的薄涂层、土壤中的次要成分或核废料蚀变产物的铀酰(VI)矿物种类。

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