Sorption of Eu(III) on Granite: EPMA, LA–ICP–MS, Batch and Modeling Studies

吸附 黑云母 化学 电子探针 离子强度 离子交换 分析化学(期刊) 无机化学 地质学 矿物学 离子 吸附 环境化学 水溶液 物理化学 石英 有机化学 古生物学
作者
Keisuke Fukushi,Yusuke Hasegawa,Koushi Maeda,Yusuke Aoi,Akihiro Tamura,Shoji Arai,Yuhei Yamamoto,Daisuke Aosai,Takashi Mizuno
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:47 (22): 12811-12818 被引量:41
标识
DOI:10.1021/es402676n
摘要

Eu(III) sorption on granite was assessed using combined microscopic and macroscopic approaches in neutral to acidic conditions where the mobility of Eu(III) is generally considered to be high. Polished thin sections of the granite were reacted with solutions containing 10 μM of Eu(III) and were analyzed using EPMA and LA-ICP-MS. On most of the biotite grains, Eu enrichment up to 6 wt % was observed. The Eu-enriched parts of biotite commonly lose K, which is the interlayer cation of biotite, indicating that the sorption mode of Eu(III) by the biotite is cation exchange in the interlayer. The distributions of Eu appeared along the original cracks of the biotite. Those occurrences indicate that the prior water-rock interaction along the cracks engendered modification of biotite to possess affinity to the Eu(III). Batch Eu(III) sorption experiments on granite and biotite powders were conducted as functions of pH, Eu(III) loading, and ionic strength. The macroscopic sorption behavior of biotite was consistent with that of granite. At pH > 4, there was little pH dependence but strong ionic strength dependence of Eu(III) sorption. At pH < 4, the sorption of Eu(III) abruptly decreased with decreased pH. The sorption behavior at pH > 4 was reproducible reasonably by the modeling considering single-site cation exchange reactions. The decrease of Eu(III) sorption at pH < 4 was explained by the occupation of exchangeable sites by dissolved cationic species such as Al and Fe from granite and biotite in low-pH conditions. Granites are complex mineral assemblages. However, the combined microscopic and macroscopic approaches revealed that elementary reactions by a single mineral phase can be representative of the bulk sorption reaction in complex mineral assemblages.
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