Geochemical characteristics of aquifer sediments and their influence on fluoride enrichment in groundwater in the Hualong-Xunhua basin

doi:10.13745/j.esf.sf.2022.9.10

Abstract

Abstract:

Natural occurrence of high-fluoride groundwater in arid and semi-arid areas seriously threatens the safety of drinking water. The chemical characteristics and formation processes of high-fluoride groundwater have been well studied, but the characteristics of high-fluoride aquifer sediments and their influence on the enrichment of groundwater fluoride remain unclear. This paper investigated the hydrogeochemical characteristics of high fluoride groundwater and the elemental compositions and water-soluble components of high-fluoride aquifer sediments to reveal how sediment geochemical characteristics affect fluoride enrichment in groundwater in the Yellow River Valley of the Hualong-Xunhua basin. The results showed that groundwater fluoride concentrations ranged from 0.51 to 3.78 mg/L (average 1.38 mg/L) and tended to increase with depth. Na⁺ was the major cation in the high fluoride groundwater and positively correlated with F^-. Total fluoride contents of sediments ranged from 460 to 1030 mg/kg, and water-soluble F^- contents ranged from 0.53 to 19.9 mg/kg. In groundwater at below fluorite saturation, a positive correlation between F^- and Ca²⁺ indicates that fluorite continues to dissolve and provides F^- to groundwater, and positive correlations between F^- and Si and F^- and Al illustrate that weathering of fluoride-containing silicate also promotes fluoride enrichment in groundwater. Positive correlations between F^- and pH, F^- and $HCO 3 -$ , and F^- and Na⁺/Ca²⁺ in both water-soluble extract of sediment and groundwater indicate that desorption and cation exchange are important hydrogeochemical processes in the formation of high-fluoride groundwater. Positive correlations between water-soluble F^- and total Fe/Mn in sediments suggest that desorbed F^- originated from Fe/Mn oxide-bound fluoride. Additionally, groundwater salinity had a positive impact on fluoride enrichment in groundwater. The results of this study are of great significance for revealing the genetic mechanisms of high fluoride groundwater.

Key words: Hualong-Xunhua basin, high fluoride groundwater, sediments, geochemical characteristics, water-rock interaction

CLC Number:

P641.3

XING Shiping, WU Ping, HU Xueda, GUO Huaming, ZHAO Zhen, YUAN Youjing. Geochemical characteristics of aquifer sediments and their influence on fluoride enrichment in groundwater in the Hualong-Xunhua basin[J]. Earth Science Frontiers, 2023, 30(2): 526-538.

Figures/Tables 10

Fig.1 The geographical location of the study area and groundwater and sediment sampling sites

Fig.2 Variation of F- and pH with depth in groundwater of the study area

Fig.4 Variations of elemental compositions (total Ca, total Mg, total Si, total Al, total Fe and total Mn) in the sediments (boreholes ZK-1, ZK-2, ZK-3, and ZK-4) with depth

Fig.5 Variations of pH and EC and component contents in water-soluble extraction of sediments (boreholes ZK-1, ZK-2, ZK-3, and ZK-4) with depth

Fig.6 Variations of total F (a) and water-soluble F- (b) in sediments (boreholes ZK-1, ZK-2, ZK-3, and ZK-4) with depth

Fig.7 Relationships between water-soluble F- content and other components in sediments (boreholes ZK-1, ZK-2, ZK-3, and ZK-4)

Fig.8 Relationships between total F- and total Ca (a), water-soluble F- and total Fe (b) and between water-soluble F- and total Mn (c) in sediments (boreholes ZK-1, Zk-2, ZK-3, and ZK-4)

Fig.3 The relationships between F- concentration and other components in groundwater of the study area

Fig.9 Relationships between F- concentration and saturation indices of calcite (a) and dolomite (b) in groundwater of the study area

Fig.10 Plots of F- concentration vs. Na+/Ca2+ ratio in groundwater (a) and water-soluble F- of sediments vs. water-soluble Na+/Ca2+ ratios of sediments (b)

References 33

[1]	RAO N S. High-fluoride groundwater[J]. Environmental Monitoring and Assessment, 2011, 176(1/2/3/4): 637-645. DOI URL
[2]	邢丽娜, 郭华明, 魏亮, 等. 华北平原浅层含氟地下水演化特点及成因[J]. 地球科学与环境学报, 2012, 34(4): 57-67.
[3]	毛若愚, 郭华明, 贾永锋, 等. 内蒙古河套盆地含氟地下水分布特点及成因[J]. 地学前缘, 2016, 23(2): 260-268. DOI
[4]	LI D N, GAO X B, WANG Y X, et al. Diverse mechanisms drive fluoride enrichment in groundwater in two neighboring sites in Northern China[J]. Environmental Pollution, 2018, 237: 430-441. DOI PMID
[5]	ALARCÓN-HERRERA M T, BUNDSCHUH J, NATH B, et al. Co-occurrence of arsenic and fluoride in groundwater of semi-arid regions in Latin America: Genesis, mobility and remediation[J]. Journal of Hazardous Materials, 2013, 262: 960-969. DOI URL
[6]	RAFIQUE T, NASEEM S, OZSVATH D, et al. Geochemical controls of high fluoride groundwater in Umarkot Sub-district, Thar Desert, Pakistan[J]. Science of the Total Environment, 2015, 530/531: 271-278. DOI URL
[7]	荆秀艳, 李小珍, 王文姬, 等. 银川平原地下水中氟分布特征及健康风险评价[J]. 环境科学与技术, 2022, 45(2): 174-181.
[8]	秦兵, 李俊霞. 大同盆地高氟地下水水化学特征及其成因[J]. 地质科技情报, 2012, 31(2): 106-111.
[9]	邢世平, 郭华明, 吴萍, 等. 化隆—循化盆地不同类型含水层组高氟地下水的分布及形成过程[J]. 地学前缘, 2022, 29(3): 115-128. DOI
[10]	ZABALA M E, MANZANO M, VIVES L. Assessment of processes controlling the regional distribution of fluoride and arsenic in groundwater of the Pampeano Aquifer in the Del Azul Creek Basin (Argentina)[J]. Journal of Hydrology, 2016, 541: 1067-1087. DOI URL
[11]	LI C C, GAO X B, WANG Y X. Hydrogeochemistry of high-fluoride groundwater at Yuncheng Basin, Northern China[J]. Science of the Total Environment, 2015, 508: 155-165. DOI URL
[12]	GUO H M, ZHANG Y, XING L N, et al. Spatial variation in arsenic and fluoride concentrations of shallow groundwater from the town of Shahai in the Hetao Basin, Inner Mongolia[J]. Applied Geochemistry, 2012, 27(11): 2187-2196. DOI URL
[13]	SU H, WANG J D, LIU J T. Geochemical factors controlling the occurrence of high-fluoride groundwater in the western region of the Ordos Basin, northwestern China[J]. Environmental Pollution, 2019, 252: 1154-1162. DOI PMID
[14]	LI Y, BI Y H, MI W J, et al. Land-use change caused by anthropogenic activities increase fluoride and arsenic pollution in groundwater and human health risk[J]. Journal of Hazardous Materials, 2021, 406: 124337. DOI URL
[15]	BURRI N M, WEATHERL R, MOECK C, et al. A review of threats to groundwater quality in the anthropocene[J]. Science of the Total Environment, 2019, 684: 136-154. DOI
[16]	SENAPATHI V, MOHAN V P, SANG Y C. GIS and geostatistical techniques for groundwater science[M]. Amsterdam:Elesver, 2019: 179-196.
[17]	KUMAR M, GOSWAMI R, PATEL A K, et al. Scenario, perspectives and mechanism of arsenic and fluoride Co-occurrence in the groundwater:a review[J]. Chemosphere, 2020, 249: 126126. DOI URL
[18]	SAXENA V, AHMED S. Dissolution of fluoride in groundwater: a water-rock interaction study[J]. Environmental Geology, 2001, 40(9): 1084-1087. DOI URL
[19]	AMINI M, MUELLER K, ABBASPOUR K C, et al. Statistical modeling of global geogenic fluoride contamination in groundwaters[J]. Environmental Science and Technology, 2008, 42(10): 3662-3668. PMID
[20]	NASEEM S, RAFIQUE T, BASHIR E, et al. Lithological influences on occurrence of high-fluoride groundwater in Nagar Parkar area, Thar Desert, Pakistan[J]. Chemosphere, 2010, 78(11): 1313-1321. DOI PMID
[21]	赵振华. 微量元素地球化学原理[M]. 2版. 北京: 科学出版社, 2016.
[22]	潘玉龙, 苏春利, 王焰新, 等. 大同盆地山阴—应县一带沉积物中氟的分布特征及控制因素[J]. 矿物岩石, 2013, 33(2): 109-114.
[23]	李亮, 吴亚, 王焰新, 等. 大同盆地地方氟病地区土壤中氟的赋存形态研究[J]. 安全与环境工程, 2014, 21(5): 52-57.
[24]	LI J X, WANG Y T, ZHU C J, et al. Hydrogeochemical processes controlling the mobilization and enrichment of fluoride in groundwater of the North China Plain[J]. Science of the Total Environment, 2020, 730: 138877. DOI URL
[25]	HE J, AN Y H, ZHANG F C. Geochemical characteristics and fluoride distribution in the groundwater of the Zhangye Basin in Northwestern China[J]. Journal of Geochemical Exploration, 2013, 135: 22-30. DOI URL
[26]	EDMUNDS W M, SMEDLEY P L. Groundwater geochemistry and health: an overview[J]. Geological Society, London, Special Publications, 1996, 113(1): 91-105. DOI URL
[27]	吴旸, 郭华明, 韩双宝, 等. 宁南西吉含水层沉积物的氟释放特征[J]. 水文地质工程地质, 2013, 40(5): 117-123.
[28]	陈劲松, 周金龙, 陈云飞, 等. 新疆喀什地区地下水氟的空间分布规律及其富集因素分析[J]. 环境化学, 2020, 39(7): 1800-1808.
[29]	XIAO J, JIN Z D, ZHANG F. Geochemical controls on fluoride concentrations in natural waters from the middle Loess Plateau, China[J]. Journal of Geochemical Exploration, 2015, 159: 252-261. DOI URL
[30]	PATEL A K, DAS N, GOSWAMI R, et al. Arsenic mobility and potential co-leaching of fluoride from the sediments of three tributaries of the Upper Brahmaputra floodplain, Lakhimpur, Assam, India[J]. Journal of Geochemical Exploration, 2019, 203: 45-58. DOI URL
[31]	GUO H M, WEN D G, LIU Z Y, et al. A review of high arsenic groundwater in Mainland and Taiwan, China: distribution, characteristics and geochemical processes[J]. Applied Geochemistry, 2014, 41: 196-217. DOI URL
[32]	GAO X B, WANG Y X, LI Y L, et al. Enrichment of fluoride in groundwater under the impact of saline water intrusion at the salt lake area of Yuncheng Basin, Northern China[J]. Environmental Geology, 2007, 53(4): 795-803. DOI URL
[33]	易春瑶, 汪丙国, 靳孟贵. 华北平原典型区土壤氟的形态及其分布特征[J]. 环境科学, 2013, 34(8): 3195-3204.