贵德盆地高氟地下水稀土元素特征及其指示意义

doi:10.13745/j.esf.sf.2022.9.3

地学前缘 ›› 2023, Vol. 30 ›› Issue (3): 505-514.DOI: 10.13745/j.esf.sf.2022.9.3

贵德盆地高氟地下水稀土元素特征及其指示意义

王振¹(), 郭华明²^,^*(), 刘海燕¹, 邢世平²

1.东华理工大学水资源与环境工程学院, 江西南昌 330032
2.中国地质大学(北京) 水资源与环境学院, 北京 100083

收稿日期:2022-06-30 修回日期:2022-08-19 出版日期:2023-05-25 发布日期:2023-04-27
通信作者: *郭华明(1975—),男,教授,主要从事水文地质学方面的教学与科研工作。E-mail: hmguo@cugb.edu.cn
作者简介:王振(1990—),男,博士,讲师,主要从事水文地球化学方面的教学与研究工作。E-mail: wzhen@ecut.edu.cn
基金资助:
国家自然科学基金项目(41222020);国家自然科学基金项目(41672225);中央高校基本科研业务费项目(2652013028);博士科研启动基金项目(DHBK2019098);博士科研启动基金项目(SHT201901);地下水循环与环境演化教育部重点实验室开放基金项目(K20220002)

Geochemical characteristics of rare earth elements in high-fluoride groundwater in the Guide Basin and its implications

WANG Zhen¹(), GUO Huaming²^,^*(), LIU Haiyan¹, XING Shiping²

1. School of Water Resources and Environment Engineering, East China University of Technology, Nanchang 330032, China
2. School of Water Resources and Environment, China University of Geosciences (Beijing), Beijing 100083, China

Received:2022-06-30 Revised:2022-08-19 Online:2023-05-25 Published:2023-04-27

摘要/Abstract

摘要：

高氟地下水是我国乃至国际社会面临的最严重的环境地质问题之一。尽管众多的研究学者已对高氟地下水形成机理开展了广泛的研究,但高氟地下水中稀土元素的分异特征和迁移规律能否指示地下水中氟的富集过程尚不完全清楚。本研究聚焦高氟地下水广泛分布的贵德盆地,通过野外调查取样、室内测试和综合分析以及水文地球化学模拟相结合的技术手段,探究了含水层中氟和稀土元素的分布特征和迁移规律。研究发现贵德盆地地下水中氟的平均浓度为2.67 mg·L^-1,75%的地下水样品中氟浓度高于1.5 mg·L^-1,且沿地下水流程呈现出上升趋势。PHREEQC计算结果表明,地下水中氟主要以自由态F^-的形式存在(浓度99.5%)。XRD 和SEM-EDS的结果表明含水层沉积物中的主要矿物为石英(含量52.9%~56.5%)和斜长石(含量19.8%~21.8%),且斜长石已发生化学风化作用。贵德盆地地下水中稀土元素浓度较低(0.052~0.267 μg·L^-1),且主要以LnCO₃⁺和Ln(CO₃)₂^-无机络合形态存在(含量>99%,Ln代表稀土元素)。地下水稀土元素北美页岩归一化模式表现为轻稀土元素相对于重稀土元素富集,且具有轻微的Ce负异常和显著的Eu正异常特征。地下水中氟和稀土元素的迁移均受到含水层中铁氧化物矿物的还原性溶解和长石类矿物的非全等水解过程的影响,且地下水中稀土元素的富集过程在一定程度上可以指示地下水中氟的富集过程。研究成果拓展了稀土元素在高氟地下水研究中的应用,可以为识别和揭示高氟地下水的分布和富集机理提供依据。

关键词: 高氟地下水, 稀土元素, 贵德盆地, 水-岩相互作用, 元素迁移和富集

Abstract:

High-fluoride groundwater is one of the most serious environmental geological problems in China and abroad. Although the formation mechanism of high-fluoride groundwater has been studied extensively by many researchers, it is not completely clear whether chemical speciation and migration characteristics of rare earth elements (REEs) in high-fluoride groundwater are indicative of the fluoride enrichment process. This study focused on the Guide Basin where high fluoride content groundwater is widely distributed, and explored the distribution and migration processes of fluoride and REEs in aquifer by field sampling, laboratory testing and comprehensive geochemical analysis, combined with hydrogeochemical simulation. It was found that the average fluoride concentration in groundwater was 2.67 mg·L^-1—with 75% of samples higher than 1.5 mg·L^-1—and showed an upward trend along the groundwater flow path. PHREEQC calculation results showed that fluoride mainly occurred as free F^- in groundwater (99.5%). XRD and SEM-EDS results showed that the main minerals in aquifer sediments were quartz (52.9%-56.5%) and plagioclase (19.8%-21.8%) that has undergone chemical weathering. REE contents in groundwater samples were low (0.052-0.267 μg·L^-1), and REEs mainly occurred as LnCO₃⁺ and Ln(CO₃)₂^- (>99%)(Ln represents REEs). NASC-normalized REE patterns showed that LREEs were enriched relative to HREEs, with slight negative Ce anomaly and obvious positive Eu anomaly. Migration of fluoride and REEs in groundwater was affected by reductive dissolution of iron oxide minerals and inhomogeneous hydrolysis of feldspar minerals, and, to certain extent, REE enrichment process was indicative of fluoride enrichment in groundwater. This research expanded REE applications in the study of high-fluoride groundwater and provided a reference for identifying high-fluoride groundwater distribution and revealing fluoride enrichment mechanisms.

Key words: high-fluoride groundwater, rare earth elements, Guide Basin, water-rock interaction, elemental migration and enrichment

中图分类号:

P641.3
P595

王振, 郭华明, 刘海燕, 邢世平. 贵德盆地高氟地下水稀土元素特征及其指示意义[J]. 地学前缘, 2023, 30(3): 505-514.

WANG Zhen, GUO Huaming, LIU Haiyan, XING Shiping. Geochemical characteristics of rare earth elements in high-fluoride groundwater in the Guide Basin and its implications[J]. Earth Science Frontiers, 2023, 30(3): 505-514.

图/表 10

图1 研究区位置及采样点分布图和AB水文地质剖面图

Fig.1 Location of the study area, distribution of sampling points in the study area, and hydrogeological profile along line AB

图2 贵德盆地地下水样品的Piper图

Fig.2 Piper plot for groundwater samples from the Guide Basin

表1 研究区地下水样品的水化学组分总表

Table 1 Summary table of hydrochemical composition of groundwater samples in the study area

水样编号	pH	Eh/ mV	ρ_B/(mg·L^-1)
水样编号	pH	Eh/ mV	TDS	NH₄-N	$H C O 3 -$	F^-	Cl^-	$N O 3 -$	$S O 4 2 -$	K⁺	Ca²⁺	Na⁺	Mg²⁺
4	8.38	110	290	0.15	221	0.77	35.6	0.00	60.6	0.99	23.3	91.8	3.83
5	8.60	145	572	0.04	92.6	3.15	225	0.67	124	2.28	14.3	196	0.07
6	8.79	142	375	0.11	166	2.23	81.4	0.24	79.6	1.47	5.44	140	0.17
8	8.55	147	639	0.21	185	3.59	218	0.42	106	2.37	8.90	236	0.33
9	8.81	99	520	0.42	299	4.08	125	0.35	68.6	2.12	4.51	212	1.11
10	8.60	99	730	0.32	312	3.62	230	0.32	91.5	3.14	7.83	280	5.08
12	9.07	116	325	0.05	117	1.85	81.4	0.32	77.4	1.13	5.86	114	0.17
13	8.97	113	365	0.05	112	1.84	101	0.84	90.8	1.08	8.65	124	0.22
19	8.74	123	482	0.08	134	2.83	155	0.35	98.6	1.69	9.27	176	0.30
20	8.70	152	475	0.09	166	3.47	127	0.23	78.1	1.39	7.66	175	0.19
21	8.90	146	538	0.012	115	2.18	145	0.57	140	1.56	8.87	191	0.42
23	8.99	195	435	0.08	115	1.32	105	0.26	137	1.15	7.85	144	0.26
24	8.95	97	510	0.12	107	2.07	135	0.32	145	1.41	8.02	174	0.40
25	8.80	143	492	0.15	156	1.90	112	0.22	139	1.55	6.62	175	0.31
32	8.87	131	540	0.36	388	5.67	90.3	0.05	104	1.88	3.44	225	0.55
34	8.82	141	572	0.34	305	4.84	98.1	0.38	104	1.78	3.76	226	0.64
35	8.70	86	623	0.585	373	5.02	121	0.40	90.4	1.93	3.97	243	1.48
41	9.08	150	365	0.25	217	1.39	46.0	0.06	86.5	1.05	3.05	127	0.32
43	8.84	29	328	0.25	188	0.86	43.8	0.47	78.7	1.13	5.87	114	0.52
44	8.70	100	315	—	171	0.66	44.2	0.44	73.9	1.21	11.0	105	1.66

表1 研究区地下水样品的水化学组分总表

Table 1 Summary table of hydrochemical composition of groundwater samples in the study area

水样编号	pH	Eh/ mV	ρ_B/(mg·L^-1)
水样编号	pH	Eh/ mV	TDS	NH₄-N	$H C O 3 -$	F^-	Cl^-	$N O 3 -$	$S O 4 2 -$	K⁺	Ca²⁺	Na⁺	Mg²⁺
4	8.38	110	290	0.15	221	0.77	35.6	0.00	60.6	0.99	23.3	91.8	3.83
5	8.60	145	572	0.04	92.6	3.15	225	0.67	124	2.28	14.3	196	0.07
6	8.79	142	375	0.11	166	2.23	81.4	0.24	79.6	1.47	5.44	140	0.17
8	8.55	147	639	0.21	185	3.59	218	0.42	106	2.37	8.90	236	0.33
9	8.81	99	520	0.42	299	4.08	125	0.35	68.6	2.12	4.51	212	1.11
10	8.60	99	730	0.32	312	3.62	230	0.32	91.5	3.14	7.83	280	5.08
12	9.07	116	325	0.05	117	1.85	81.4	0.32	77.4	1.13	5.86	114	0.17
13	8.97	113	365	0.05	112	1.84	101	0.84	90.8	1.08	8.65	124	0.22
19	8.74	123	482	0.08	134	2.83	155	0.35	98.6	1.69	9.27	176	0.30
20	8.70	152	475	0.09	166	3.47	127	0.23	78.1	1.39	7.66	175	0.19
21	8.90	146	538	0.012	115	2.18	145	0.57	140	1.56	8.87	191	0.42
23	8.99	195	435	0.08	115	1.32	105	0.26	137	1.15	7.85	144	0.26
24	8.95	97	510	0.12	107	2.07	135	0.32	145	1.41	8.02	174	0.40
25	8.80	143	492	0.15	156	1.90	112	0.22	139	1.55	6.62	175	0.31
32	8.87	131	540	0.36	388	5.67	90.3	0.05	104	1.88	3.44	225	0.55
34	8.82	141	572	0.34	305	4.84	98.1	0.38	104	1.78	3.76	226	0.64
35	8.70	86	623	0.585	373	5.02	121	0.40	90.4	1.93	3.97	243	1.48
41	9.08	150	365	0.25	217	1.39	46.0	0.06	86.5	1.05	3.05	127	0.32
43	8.84	29	328	0.25	188	0.86	43.8	0.47	78.7	1.13	5.87	114	0.52
44	8.70	100	315	—	171	0.66	44.2	0.44	73.9	1.21	11.0	105	1.66

图3 水化学成分和不同形态氟沿流程的变化

Fig.3 Variation trends of ∑REE and water-quality parameters along the flow path (top panel) and percentage variations of different forms of fluoride along the flow path and with pH (bottom panel)

图4 光学显微镜下18.8 m、104 m和362 m深度含水层沉积物的主要矿物组成照片(a,b,c)及362 m深度沉积物的SEM-EDS图(d) Pl、Qtz、Ab和Hm分别表示斜长石、石英、钠长石、赤铁矿。图d中,cps表示每秒的计数,cps/keV和cps/eV分别表示每千电子伏特和每电子伏特下能谱仪每秒所收集到的反射粒子数。

Fig.4 Main minerals identified in aquifer sediments at depths of (a) 18.8 m, (b) 104 m and (c) 362 m under optical microscope, and (d) SEM-EDS analysis results on sediment at depth of 362 m. Pl, Qtz, Ab and Hm represent plagioclase, quartz, albitite and hematite, respectively.

表2 贵德盆地地下水中稀土元素浓度

Table 2 Descriptive statistics of raw data on REE contents in groundwater of the Guide Basin

统计量	ρ_B/(ng·L^-1)
统计量	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu
最小值	6	9	1.21	4.5	1.18	2.11	2.09	0.18	0.98	0.21	0.76	0.07	0.56	0.00
最大值	50	92	20.7	88.7	14.3	30.5	13.1	1.52	6.87	1.47	3.62	0.73	3.48	0.68
平均值	22	39	6.84	26.2	4.74	10.6	5.37	0.58	3.03	0.65	1.83	0.28	1.57	0.18
标准差	12	21	4.44	19.0	3.11	6.59	2.85	0.36	1.88	0.30	0.82	0.19	0.75	0.15

图5 不同水化学成分的相关关系图 a—∑REE浓度与Eh关系图;b—∑REE浓度与Fe浓度关系图;c—∑REE浓度与pH关系图;d— H C O 3 -浓度与NH4-N浓度关系图。

Fig.5 Scatter plots showing correlation between (a) ∑REE and Eh, (b) ∑REE and Fe, (c) ∑REE and pH, and (d) NH4-N and HCO3-

图6 LnCO3+ (a)和Ln(CO3)2- (b)形态的稀土元素占比沿流程的变化

Fig.6 Changes in the proportion of (a) LnCO3+ and (b) Ln(CO3)2- in groundwater along the flow path

图7 地下水中稀土元素的配分模式

Fig.7 NASC-normalized REE distribution patterns in groundwater samples

图8 不同水化学成分的相关关系图 a—∑REE浓度与Na+浓度关系图;b—Sr/Ca与HCO3-浓度关系图;c—Na/Ca与F-浓度关系图;d—∑REE浓度与F-浓度关系图。

Fig.8 Scatter plots showing correlation between (a) ∑REE and Na+, (b) Sr/Ca and HCO3-, (c) Na/Ca and F-, and (d) ∑REE and F-

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贵德盆地高氟地下水稀土元素特征及其指示意义

Geochemical characteristics of rare earth elements in high-fluoride groundwater in the Guide Basin and its implications

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