Distribution and fractionation of rare earth elements in high fluoride groundwater from the North China Plain

被引：0
作者：
Liu H. [1 ,2 ]
Liu M. [1 ,2 ]
Zhang W. [1 ,2 ]
Sun Z. [1 ,2 ]
Wang Z. [1 ,2 ]
Wu T. [1 ,2 ]
Guo H. [3 ]
机构：
[1] State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang
[2] School of Water Resources and Environmental Engineering, East China University of Technology, Nanchang
[3] School of Water Resources and Environment, China University of Geosciences(Beijing), Beijing
来源：
Earth Science Frontiers | 2022年 / 29卷 / 03期
关键词：
Elemental migration and transformation; Enrichment and fractionation; Hydrochemistry; North China Plain; Water-rock interactions;
D O I：
10.13745/j.esf.sf.2021.7.24
中图分类号：
学科分类号：
摘要：
High-fluoride groundwater is a major environmental problem that has caused global concerns. Although numerous studies have been done on the chemical characteristics, formation and migration mechanisms of high-fluoride groundwater, little is known about the concentrations and fractionation characteristics of rare earth elements (REE) in high-fluoride groundwater or if REE can be used as a tracer for studying the formation and distribution of high-fluoride groundwater. These uncertainties have limited REE application in high-fluoride groundwater research. In this paper, we investigated the fluoride and REE concentrations and distributions in groundwater collected along a flow path in the North China Plain (NCP) where strong fluoride anomalies in groundwater were observed. We found the groundwater fluoride concentrations ranged from 0.28 to 9.33 mg/L, with 55% groundwater exceeding the China drinking water standard (1 mg/L). According to PHREEQC calculation, fluorine occurs in groundwater as NaF, CaF+, MgF+ and, predominantly, F-(85.42%-99.39%). High-fluoride groundwater is mainly distributed in the central alluvial lacustrine plain and the eastern alluvial marine plain, with 60% at depths below 180 m. Hydrochemical analysis indicated the formation of shallow high-fluoride groundwater is mainly controlled by evaporation and concentration, while deep high-fluoride groundwater is a result of mineral dissolution and competitive ion adsorption through water-rock interactions. The groundwater REE concentration is at pico to nanomolar level, and, according to PHREEQC calculation, REE species are mainly carbonate complexes (REECO3+ and REE(CO3)2-), with 0-1.18% REE in complex with F-(REEF2+ and REEF2+). The upper continental crust (UCC)-normalized REE patterns are characterized by enrichments of heavy REE (HREE) and middle REE (MREE) over light REE (LREE) and have significant negative Ce anomalies (0.11<Ce/Ce*=CeUCC/(LaUCC×PrUCC)0.5<2.29). The HREE enrichment in groundwater is mainly attributed to the preferential complexation of HREE over LREE or HREE with carbonate in forming more stable carbonate complexes. Along a groundwater flow path, both REE and fluoride concentrations in deep aquifers generally increase following similar trends. Besides, high-fluoride groundwater is more prone to HREE enrichment. These findings suggest that REE can potentially be used as a fluoride indicator for studying fluoride enrichment in natural aquifer systems. © 2022, Editorial Office of Earth Science Frontiers. All right reserved.
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页码：129 / 144
页数：15
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