华北平原高氟地下水中稀土元素分布和分异特征

doi:10.13745/j.esf.sf.2021.7.24

地学前缘 ›› 2022, Vol. 29 ›› Issue (3): 129-144.DOI: 10.13745/j.esf.sf.2021.7.24

华北平原高氟地下水中稀土元素分布和分异特征

刘海燕¹^,²(), 刘茂涵¹^,², 张卫民¹^,², 孙占学¹^,², 王振¹^,², 吴通航¹^,², 郭华明³^,^*()

1.东华理工大学核资源与环境国家重点实验室, 江西南昌 330032
2.东华理工大学水资源与环境工程学院, 江西南昌 330032
3.中国地质大学(北京) 水资源与环境学院, 北京 100083

收稿日期:2021-04-28 修回日期:2021-06-30 出版日期:2022-05-25 发布日期:2022-04-28
通信作者: 郭华明
作者简介:刘海燕(1988—),男,博士,讲师,主要从事水文地球化学研究。E-mail: hy_liu@ecut.edu.com
基金资助:
国家自然科学基金项目(41902243);国家自然科学基金项目(41222020);国家自然科学基金项目(41672225);中国霍英东教育基金项目(131017);中国地质调查局地调项目(12120113103700);东华理工大学博士科研启动基金项目(DHBK2019094);东华理工大学博士科研启动基金项目(SHT201901)

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

LIU Haiyan¹^,²(), LIU Maohan¹^,², ZHANG Weimin¹^,², SUN Zhanxue¹^,², WANG Zhen¹^,², WU Tonghang¹^,², GUO Huaming³^,^*()

1. State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang 330032, China
2. School of Water Resources and Environmental Engineering, East China University of Technology, Nanchang 330032, China
3. School of Water Resources and Environment, China University of Geosciences(Beijing), Beijing 100083, China

Received:2021-04-28 Revised:2021-06-30 Online:2022-05-25 Published:2022-04-28
Contact: GUO Huaming

摘要/Abstract

摘要：

高氟地下水是世界各国研究者广泛关注的重大环境问题。尽管对高氟地下水的化学特征、形成机理和扩散机制等已有不少研究,但其稀土元素(REE)的含量和分异特征以及这些特征能否反映高氟地下水的形成和分布尚不清楚,这在一定程度上限制了REE在高氟地下水中的运用。本研究以地下水氟离子异常严重地区——华北平原为研究区,沿地下水流向采集浅层和深层地下水样,研究分析了水中氟离子和REE的地球化学特征。浓度分析结果表明地下水氟离子浓度介于0.28 mg/L和9.33 mg/L之间,其中55%超出我国饮用水标准规定值1.0 mg/L;PHREEQC计算结果反映地下水中氟以NaF、CaF⁺、MgF⁺和自由态F^-形式存在,其中自由态F^-含量占主导(85.42%99.39%);高氟地下水主要分布于中部冲积湖积平原以及东部冲积海积平原,60%高氟地下水样分布在180 m深度以下;水化学图件分析结果指示浅层高氟地下水的形成主要受蒸发浓缩作用的控制,而深层高氟地下水是水岩相互作用下的矿物溶解和离子竞争吸附共同作用的结果。研究区地下水REE含量处于pmol/L至nmol/L级别,PHREEQC模拟计算结果表明REE主要以碳酸络合物( $REECO 3 +$ 和$REE(CO_{3})_{2}^{-})$的形式存在,与氟离子络合的稀土元素(REEF²⁺和 $REEF 2 +$ )占01.18%;上陆壳(UCC)标准化结果显示,所有地下水均呈重REE(HREE)和中REE(MREE)相对于轻REE(LREE)富集的模式,且具有显著Ce负异常(0.11<Ce/Ce^* = Ce_UCC/(La_UCC×Pr_UCC)^0.5<2.29)特性;地下水富HREE主要归因于HREE比LREE优先与碳酸根络合,并且形成更加稳定的碳酸络合物。沿地下水流向,深层地下水中总REE含量与地下水中氟浓度均呈现不断上升的变化趋势,同时高氟地下水比低氟地下水更易富集重稀土元素,说明稀土元素对深层含水层富氟行为具有一定的指示作用。

关键词: 水文地球化学, 水岩相互作用, 元素迁移转化, 富集分异, 华北平原

Abstract:

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 ( $REECO 3 +$ and $REE(CO_{3})_{2}^{-})$, with 0-1.18% REE in complex with F^-(REEF²⁺ and $REEF 2 +$ ). 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^*=Ce_UCC/(La_UCC×Pr_UCC)^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.

Key words: hydrochemistry, water-rock interactions, elemental migration and transformation, enrichment and fractionation, North China Plain

中图分类号:

P641.3
P595

刘海燕, 刘茂涵, 张卫民, 孙占学, 王振, 吴通航, 郭华明. 华北平原高氟地下水中稀土元素分布和分异特征[J]. 地学前缘, 2022, 29(3): 129-144.

LIU Haiyan, LIU Maohan, ZHANG Weimin, SUN Zhanxue, WANG Zhen, WU Tonghang, GUO Huaming. Distribution and fractionation of rare earth elements in high fluoride groundwater from the North China Plain[J]. Earth Science Frontiers, 2022, 29(3): 129-144.

图/表 16

图1 华北平原地理位置及第四纪地貌图

Fig.1 Geographical location of and Quaternary landforms in the North China Plain

图2 研究区地下水采样点分布图

Fig.2 Distribution of groundwater sampling locations in the study area

表1 WATEQ4F中用于模拟氟阳离子络合的反应式及平衡常数

Table 1 Chemical equations and equilibrium constants used for simulating F--cation complexation reactions in WATEQ4F

反应	平衡常数	参考文献
Mg²⁺ + F^- = MgF⁺	1.82	[22]
Ca²⁺+ F^- = CaF⁺	0.94	[22]
Na⁺ + F^- = NaF	-0.24	[22]
Al³⁺ + F^- = AlF²⁺	7.0	[23]
Al³⁺ + 2F^- = Al $F 2 +$	12.7	[23]
Al³⁺ + 3F^- = AlF₃	16.8	[23]
Al³⁺ + 4F^- = Al $F 4 -$	19.4	[23]
Fe³⁺ + F^- = FeF²⁺	6.2	[22]
Fe³⁺ + 2F^- = Fe $F 2 +$	10.8	[22]
Fe³⁺ + 3F^- = FeF₃	14	[22]

表1 WATEQ4F中用于模拟氟阳离子络合的反应式及平衡常数

Table 1 Chemical equations and equilibrium constants used for simulating F--cation complexation reactions in WATEQ4F

反应	平衡常数	参考文献
Mg²⁺ + F^- = MgF⁺	1.82	[22]
Ca²⁺+ F^- = CaF⁺	0.94	[22]
Na⁺ + F^- = NaF	-0.24	[22]
Al³⁺ + F^- = AlF²⁺	7.0	[23]
Al³⁺ + 2F^- = Al $F 2 +$	12.7	[23]
Al³⁺ + 3F^- = AlF₃	16.8	[23]
Al³⁺ + 4F^- = Al $F 4 -$	19.4	[23]
Fe³⁺ + F^- = FeF²⁺	6.2	[22]
Fe³⁺ + 2F^- = Fe $F 2 +$	10.8	[22]
Fe³⁺ + 3F^- = FeF₃	14	[22]

表2 加入至PHREEQC数据库WATEQ4F中的稀土元素与阴离子络合反应稳定参数(离子强度IS=0,温度25℃,REE代表稀土元素)

Table 2 Chemical equations and equilibrium constants added to the WATEQ4F database in PHREEQC calculation for REE- anion complexation reactions (ionic strength, 0; temperature, 25℃)

表3 研究区地下水化学组分统计表

Table 3 Statistical table of chemical composition of groundwater in three study zones

区域	统计量		pH		地下水中各化学组分的指标参数统计值
区域	统计量		pH		TDS		$HCO 3 -$		Cl^-		$NO 3 -$	$SO 4 2 -$	F^-	K⁺	Na⁺	Ca²⁺	Mg²⁺
一区	最大值	7.97		963.00		461.16		376.63		115.85		76.08	1.33	1.86	37.49	220.71	68.14
	最小值	7.10		222.00		204.96		3.60		0.00		11.99	0.28	0.05	3.55	<检出限	24.55
	平均值	7.64		391.61		302.15		48.78		44.49		43.17	0.70	1.23	11.69	91.14	31.77
	标准差	0.20		155.61		65.88		83.97		37.81		17.98	0.24	0.53	7.06	43.04	9.61
	变异系数	0.03		0.40		0.22		1.72		0.85		0.42	0.34	0.43	0.60	0.47	0.30
二区	最大值	8.80		4 349.00		924.76		984.36		123.16		2 890.38	7.07	5.66	973.42	333.18	476.73
	最小值	7.08		274.00		31.72		4.71		0.44		17.99	0.71	0.33	28.14	3.59	1.50
	平均值	7.96		1 031.38		438.27		209.92		8.84		395.00	2.91	1.35	261.08	81.93	72.75
	标准差	0.55		1 047.07		193.14		263.43		27.14		735.41	1.81	1.26	234.02	98.49	113.32
	变异系数	0.07		1.02		0.44		1.25		3.07		1.86	0.62	0.93	0.90	1.20	1.56
三区	最大值	8.51		1 179.00		405.04		463.45		5.77		242.52	9.33	2.60	429.25	13.87	14.41
	最小值	8.20		796.00		275.72		56.01		1.72		40.70	1.39	0.76	277.00	7.32	1.62
	平均值	8.42		996.80		340.14		292.06		3.52		122.18	5.12	1.59	361.71	10.27	5.81
	标准差	0.12		132.50		41.77		134.64		1.58		94.54	2.87	0.60	52.50	2.24	4.44
	变异系数	0.01		0.13		0.12		0.46		0.45		0.77	0.56	0.37	0.15	0.22	0.76

表3 研究区地下水化学组分统计表

Table 3 Statistical table of chemical composition of groundwater in three study zones

区域	统计量		pH		地下水中各化学组分的指标参数统计值
区域	统计量		pH		TDS		$HCO 3 -$		Cl^-		$NO 3 -$	$SO 4 2 -$	F^-	K⁺	Na⁺	Ca²⁺	Mg²⁺
一区	最大值	7.97		963.00		461.16		376.63		115.85		76.08	1.33	1.86	37.49	220.71	68.14
	最小值	7.10		222.00		204.96		3.60		0.00		11.99	0.28	0.05	3.55	<检出限	24.55
	平均值	7.64		391.61		302.15		48.78		44.49		43.17	0.70	1.23	11.69	91.14	31.77
	标准差	0.20		155.61		65.88		83.97		37.81		17.98	0.24	0.53	7.06	43.04	9.61
	变异系数	0.03		0.40		0.22		1.72		0.85		0.42	0.34	0.43	0.60	0.47	0.30
二区	最大值	8.80		4 349.00		924.76		984.36		123.16		2 890.38	7.07	5.66	973.42	333.18	476.73
	最小值	7.08		274.00		31.72		4.71		0.44		17.99	0.71	0.33	28.14	3.59	1.50
	平均值	7.96		1 031.38		438.27		209.92		8.84		395.00	2.91	1.35	261.08	81.93	72.75
	标准差	0.55		1 047.07		193.14		263.43		27.14		735.41	1.81	1.26	234.02	98.49	113.32
	变异系数	0.07		1.02		0.44		1.25		3.07		1.86	0.62	0.93	0.90	1.20	1.56
三区	最大值	8.51		1 179.00		405.04		463.45		5.77		242.52	9.33	2.60	429.25	13.87	14.41
	最小值	8.20		796.00		275.72		56.01		1.72		40.70	1.39	0.76	277.00	7.32	1.62
	平均值	8.42		996.80		340.14		292.06		3.52		122.18	5.12	1.59	361.71	10.27	5.81
	标准差	0.12		132.50		41.77		134.64		1.58		94.54	2.87	0.60	52.50	2.24	4.44
	变异系数	0.01		0.13		0.12		0.46		0.45		0.77	0.56	0.37	0.15	0.22	0.76

图3 研究区水样piper三线图

Fig.3 Piper plot for groundwater samples from the study area

图4 水化学Gibbs图

Fig.4 Gibbs diagram for groundwater samples

图5 研究区地下水氟浓度空间分布

Fig.5 (a) Horizontal distribution and (b) depth dependence of F- concentration in groundwater in the study area

图6 地下水中pH与氟形态比例(a)和氟离子浓度(b)之间的变化关系

Fig.6 Relationship between pH and fluorine species percentage (a) or total F- concentration (b) in groundwater

表4 研究区稀土元素含量及分异特征参数

Table 4 REE concentrations and fractionation parameters in groundwater collected from the North China Plain (NCP)

区域	统计量		元素含量/(pmol·L^-1)
区域	统计量		La	Ce	Pr		Nd	Sm		Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu
一区	最小值		40	20	6		27	10		85	14	1	2	1	3	0	2	1
	最大值		242	444	57		218	38		589	43	7	44	13	45	9	65	13
	平均值		124	135	24		102	22		209	26	3	19	5	16	2	16	3
二区	最小值		36	27	6		16	8		18	10	1	5	1	4	1	2	1
	最大值		982	1 503	273		835	342		559	404	49	224	32	85	13	61	14
	平均值		212	306	46		171	45		197	51	6	33	7	20	3	18	4
三区	最小值		35	70	12		42	7		85	11	1	6	4	5	1	5	1
	最大值		1 648	2 545	377		1 471	282		309	291	38	183	39	109	16	95	16
	平均值		514	822	120		471	91		181	89	12	60	13	36	5	29	5
区域		统计量	元素含量/(pmol·L^-1)								(La/Sm)_UCC		(Gd/Yb)_UCC		Ce/Ce^*		Eu/Eu^*
区域		统计量	∑REE			∑LREE			∑HREE		(La/Sm)_UCC		(Gd/Yb)_UCC		Ce/Ce^*		Eu/Eu^*
一区		最小值	392			368			23		0.48		0.33		0.11		19.03
		最大值	1 176			1 039			236		1.08		3.51		2.29		89.81
		平均值	707			617			90		0.8		1.2		0.61		43.52
二区		最小值	174			113			31		0.33		0.22		0.31		2.27
		最大值	4 631			3 786			846		2.77		4.26		1.52		90.62
		平均值	1 119			977			142		0.74		1.62		0.8		43.04
三区		最小值	286			251			35		0.73		1.14		0.74		2.56
		最大值	7 266			6 480			786		0.81		1.82		0.81		45.79
		平均值	2 447			2 198			249		0.76		1.49		0.77		22.28

图7 研究区地下水Nd、∑REE含量变化图(a)以及∑REE含量随深度变化图(b)

Fig.7 Horizontal variations of Nd content and ∑REE (a) and vertical variation of ∑REE (b) in groundwater in the study area

图8 研究区地下水Nd、Sm、Yb元素形态模拟结果 a,b,c为浅层地下水;d,e,f为深层地下水。

Fig.8 Simulated Nd, Sm and Yb speciations in shallow (a, b, c) and deep (d, e, f) groundwater in the study area

图9 研究区地下水平均上陆壳标准化稀土元素配分模式 a,b,c分别为一区、二区、三区情况;d为Ce异常和Eu异常的变化情况。

Fig.9 UCC-normalized REE pattern for groundwater in study zones I-III (a-c) and horizontal variations of Ce/Ce* and Eu/Eu* (d) in groundwater in the study area

图10 研究区地下水中Eh值与Ce/Ce*(a)、Eu/Eu*(b)之间的变化关系

Fig.10 Relationship between Eh and Ce/Ce* (a) or Eu/Eu* (b) in groundwater in the study area

图11 研究区地下水中F-浓度与∑REE含量(a)、(La/Sm)UCC(b)之间的变化关系

Fig.11 Relationship between F- concentration and ∑REE (a) or (La/Sm)UCC (b) in groundwater in the study area

图12 研究区地下水中 HCO 3 -浓度与F-浓度之间的变化关系(a)和稀土元素碳酸根络合反应稳定平衡常数(K)随原子序数的变化(b)(图b数据来源文献[26,28,39⇓-41])

Fig.12 (a) Relationship between HCO 3 - and F- in groundwater and (b) variation of equilibrium constants for REE-carbonate complexation reactions with increasing atomic number (data from [26,28,39⇓-41])

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华北平原高氟地下水中稀土元素分布和分异特征

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

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