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碱性环境中氢氧化镁颗粒及与胶体相关的152铕:存在和不存在碳酸盐时的胶体表征及吸附特性

Magnesium hydroxide bulk and colloid-associated 152Eu in an alkaline environment: colloid characterisation and sorption properties in the presence and absence of carbonate.

作者信息

Pitois Aurelien, Ivanov Peter I, Abrahamsen Liam G, Bryan Nick D, Taylor Robin J, Sims Howard E

机构信息

University of Manchester, Centre for Radiochemistry Research, Oxford Road, Manchester, UKM13 9PL.

出版信息

J Environ Monit. 2008 Mar;10(3):315-24. doi: 10.1039/b714636c. Epub 2008 Jan 14.

DOI:10.1039/b714636c
PMID:18392273
Abstract

The distribution of 152Eu between magnesium hydroxide bulk, colloids and solution has been assessed under alkaline conditions, such as those in nuclear fuel storage ponds. The colloidal phase has been characterised by two complementary methods: coupled ultrafiltration-ICP-AES and scanning electron microscopy. The quantity and the size distribution of the colloidal phase is strongly ionic strength-dependent. A decrease of the quantity of colloids, in particular the larger size ranges, has been observed with increasing ionic strength. Small colloids (1 kDa-10 kDa fraction) are predominant at all ionic strengths. The morphology of colloids, observed by field-emission gun scanning electron microscopy, appears to change from hexagonal prismatic (characteristic to the mineral) to spherical (energetically more favourable) as size decreases. The distribution of 152Eu between the solid and liquid/colloidal phases has been investigated at carbonate concentrations ranging from 0 to 10(-2) M by coupled ultrafiltration and gamma-spectrometry. Mg(OH)2 bulk appears to be a very strong sorbent for 152Eu, since complete sorption onto the bulk happens for carbonate concentrations as high as 10(-3) M. Scavenging of 152Eu by Mg(OH)2 colloids is negligible in the presence of Mg(OH)2 bulk. The distribution of 152Eu between liquid and colloidal phases has been investigated in the absence of bulk at various carbonate concentrations. A significant uptake of 152Eu by the colloids in solution has been observed, which decreases with increasing carbonate concentration. 152Eu appears to be mainly associated to the smallest colloids (1 kDa-10 kDa fraction). There is a strong correlation between the sorption properties and the surface area of the colloids.

摘要

已在碱性条件下(如核燃料储存池中的条件)评估了152铕在氢氧化镁本体、胶体和溶液之间的分布情况。通过两种互补方法对胶体相进行了表征:耦合超滤 - 电感耦合等离子体发射光谱法和扫描电子显微镜法。胶体相的数量和尺寸分布强烈依赖于离子强度。随着离子强度增加,已观察到胶体数量减少,特别是较大尺寸范围的胶体。在所有离子强度下,小胶体(1 kDa - 10 kDa部分)占主导地位。用场发射枪扫描电子显微镜观察到,随着尺寸减小,胶体的形态似乎从六方棱柱形(矿物的特征形态)变为球形(能量上更有利)。通过耦合超滤和伽马能谱法,研究了在碳酸盐浓度范围为0至10^(-2) M时152铕在固相与液相/胶体相之间的分布。氢氧化镁本体似乎是152铕的极强吸附剂,因为在碳酸盐浓度高达10^(-3) M时,152铕会完全吸附到本体上。在存在氢氧化镁本体的情况下,氢氧化镁胶体对152铕的清除作用可忽略不计。在不存在本体的情况下,研究了在各种碳酸盐浓度下152铕在液相和胶体相之间的分布。已观察到溶液中的胶体对152铕有显著吸收,且随着碳酸盐浓度增加而降低。152铕似乎主要与最小的胶体(1 kDa - 10 kDa部分)相关。吸附特性与胶体的表面积之间存在很强的相关性。

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