华北平原原生富碘地下水系统中碘的迁移富集规律:以石家庄-衡水-沧州剖面为例

薛肖斌; 李俊霞; 钱坤; 谢先军

doi:10.3799/dqkx.2017.564

华北平原原生富碘地下水系统中碘的迁移富集规律:以石家庄-衡水-沧州剖面为例

doi: 10.3799/dqkx.2017.564

薛肖斌^1,2,,
李俊霞^1,2,3, ,,
钱坤^1,2,
谢先军^1,2,3

1.
中国地质大学环境学院, 湖北武汉 430074
2.
中国地质大学生物地质与环境地质国家重点实验室, 湖北武汉 430074
3.
中国地质大学盆地水文学与湿地生态恢复实验室, 湖北武汉 430074

基金项目:

国家自然科学基金项目 41502230

详细信息

作者简介:
薛肖斌(1992-), 男, 硕士研究生, 主要从事地下水污染与防治方面的研究工作

通讯作者:
李俊霞

中图分类号: P641.1
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- 被引次数: 0
出版历程
- 收稿日期: 2017-12-03
- 刊出日期: 2018-03-15

Spatial Distribution and Mobilization of Iodine in Groundwater System of North China Plain: Taking Hydrogeological Section from Shijiazhuang, Hengshui to Cangzhou as an Example

Xue Xiaobin^{1,2
,},
Li Junxia^{1,2,3
, ,},
Qian Kun^1,2,
Xie Xianjun^1,2,3

1.
School of Environmental Studies, China University of Geosciences, Wuhan 430074, China
2.
State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074, China
3.
Laboratory of Basin Hydrology and Wetland Eco-Restoration, China University of Geosciences, Wuhan 430074, China

摘要

摘要: 高碘地下水是继高砷、高氟地下水之后的又一全球性饮水安全问题，但对地下水系统中碘的赋存形态及迁移富集机理研究尚显不足.为了解华北平原地下水系统中碘的空间分布特征及迁移富集规律，选取石家庄-衡水-沧州典型水文地质剖面，完成地下水样品采集，分析其水化学组成、总碘含量及碘形态组成特征，同时运用phreeqc完成水文地质剖面地球化学反向模拟及相关矿物饱和指数计算，定性定量表征水流场内所发生的水文地球化学过程，进而深入探讨上述过程对地下水系统碘迁移富集的影响.结果表明，区域内地下水中碘含量变化范围为3.35~1 106.00 μg/L，其中，41.86%样品碘含量超过《水源性高碘地区和地方性高碘甲状腺肿病区的规定（GB/T19380-2003）》所界定的150 μg/L国家标准；空间上，高碘地下水主要分布于渤海湾区；地下水中碘的主要赋存形态为碘离子及碘酸根离子，其分布受氧化还原环境控制，碘酸根离子主要出现于氧化环境中；沿地下水流向，地下水环境朝利于液相碘迁移富集的方向演变；渤海湾区，海水入侵影响下形成的偏碱性、（弱）还原环境，利于碘从沉积物中迁移释放至地下水中；碘在不同铁矿物相上的搭载能力及氧化还原环境演化导致的铁矿物相转化，是造成华北平原地下水系统中碘迁移富集的主要水文地球化学过程.
- 碘 /
- 迁移富集 /
- 地下水 /
- 华北平原
Abstract: High iodine groundwater is another global drinking water safety problem in addition to after high arsenic and high fluorine groundwater. However, the research on the existing forms of iodine and the mechanisms of migration and enrichment of iodine in groundwater system is still insufficient research on the existing forms of iodine and the mechanisms of migration and enrichment of iodine in groundwater system. To understand spatial distribution and mobilization of iodine in groundwater system of North China plain(NCP), a hydrochemical study was conducted. The results show that iodine concentration in groundwater from NCP rangesd from 3.35 to 1 106 μg/L, and 41.86% of groundwater samples has iodine concentration exceeding drinking water level (150 μg/L) recommended by Chinese government. High iodine groundwater (>150 μg/L) is mainly distributed in deep aquifers of Bohai bay area. The main species of groundwater iodine include mainly diodide and iodate, the distribution of which is controlled by redox environment of groundwater, and iodate mainly occurs in oxidizing condition. Along the groundwater flow path from Shijiazhuang, Hengshui to Cangzhou, hydrochemical evolution and inverse modeling were performed to understand the groundwater environment favoring iodine enrichment in groundwater. The results of hydrochemical evolution showed that at Bohai bay area, the weak-alkalinity and (sub)reducing environment influenced by seawater intrusion favor the iodine release and enrichment in groundwater.The adsorption equilibration of iodine among metal oxyhydroxides under various environments is the primary hydrogeochemical process controlling iodine mobilization in the groundwater system of the North China plain.
- iodine /
- mobilization /
- groundwater /
- North China Plain

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图 1 研究区采样点位置与地下水碘含量概况

Fig. 1. Sampling location of groundwater samples from NCP

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图 2 地下水中碘含量与井深关系

▲：Ⅰ区补给区；■：Ⅱ区径流区；●：Ⅲ区排泄及海水入侵区

Fig. 2. Depth profile of iodine concentrations in groundwater samples from NCP

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图 3 碘形态相对含量图

Fig. 3. Ternary diagram of iodine species in groundwater

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图 4 Piper三线图

△代表Ⅰ区补给区；□代表Ⅱ区径流区；○代表Ⅲ区排泄及海水入侵区

Fig. 4. Piper diagram of groundwater samples from NCP

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图 5 剖面总碘含量、Cl/Br摩尔比、Cl/(Cl+HCO₃)质量比和pH演化图

Fig. 5. The variations of groundwater iodine, Cl/Br molar ratio, Cl/(Cl+HCO₃) weight ratio and pH along groundwater flow path from Shijiazhuang/Hengshui to Cangzhou

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图 6 碘含量与pH(a)、Eh(b)、Fe(c)、HCO₃(d)的关系图

▲：Ⅰ区补给区；■：Ⅱ区径流区；●：Ⅲ区排泄及海水入侵区

Fig. 6. The plots of groundwater iodine vs. pH (a), Eh (b), Fe (c) and HCO₃ (d)

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表 1 华北平原第四系地层、岩性、含水层组和海侵划分

Table 1. Events of Quaternary marine transgressions at North China Plain (NCP)

	符号	岩性描述	底界埋深	总厚度	含水层组	海侵
全新统	Q4	含淤泥质粉土、粉质粘土夹细砂粉砂	15~30 m，局部为60~70 m	20~30 m	第1含水层组	天津海侵
上更新统	Q3	粉土、粉质粘土、粉细砂、中细砂、卵石	10~170 m	50~150 m	第2含水层组	白洋淀、沧州海侵
中更新统	Q2	粉质粘土夹砂、砾石	250~350 m	80~180 m	第3含水层组	海兴、黄骅海侵
下更新统	Q1	厚层粘土、粉质粘土夹砂	350~550 m	100~200 m	第4含水层组	渤海海侵

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表 2 样品数据统计

Table 2. Statistical description of chemical composition of groundwater samples from NCP

	Ⅰ区					Ⅱ区					Ⅲ区
	最小值	最大值	平均值	中位数	标准差	最小值	最大值	平均值	中位数	标准差	最小值	最大值	平均值	中位数	标准差
总碘(μg/L)	3.35	20.99	8.82	7.23	5.03	7.66	138.00	54.12	37.74	41.82	197.80	1 106.00	598.00	546.40	282.20
碘酸根(μg/L)	ND	17.63	3.26	2.18	5.21	ND	115.50	16.24	ND	32.42	ND	694.60	134.80	3.88	228.50
碘离子(μg/L)	0.87	11.56	2.24	1.11	3.30	0.70	91.21	29.50	16.12	29.80	34.47	854.00	424.80	358.30	259.80
有机碘(μg/L)	2.07	5.91	3.32	2.83	1.16	ND	20.2	8.65	7.01	6.92	-17.19	296.10	43.63	4.98	85.14
pH	7.25	8.36	7.62	7.49	0.38	7.64	8.55	8.16	8.16	0.21	7.80	8.34	8.048	8.10	0.15
TDS(mg/L)	269.5	817.7	461.9	309.2	222.3	391.1	866.4	671.2	702.8	158.4	892.0	2 400.0	1 480.0	1 498.0	373.4
Eh(mV)	122.00	170.00	145.60	148.00	17.08	86.00	135.00	113.70	115.00	15.96	-214.00	126.00	-2.221	51.55	132.60
F(mg/L)	0.19	0.67	0.41	0.42	0.14	0.43	3.37	1.51	1.31	1.01	1.93	4.89	3.03	2.74	0.75
Cl/Br (摩尔比)	132.5	3 677.0	938.0	706.4	1 069.0	381.2	2 937.0	1 305.0	1 270.0	570.0	582.3	2 465.0	1 391.0	1 348.0	548.6
Cl(mg/L)	7.16	64.33	33.16	32.99	25.00	11.90	263.00	107.20	113.20	60.91	110.10	705.00	381.50	388.00	153.30
NO₃(mg/L)	2.000	139.500	31.150	8.050	43.450	ND	7.050	0.900	ND	1.870	ND	5.580	1.074	ND	1.970
SO₄(mg/L)	23.12	200.80	90.60	53.95	72.90	67.47	273.80	152.40	146.00	44.74	87.26	277.70	170.00	158.00	55.48
HCO₃(mg/L)	188.50	400.80	293.00	289.70	64.57	91.50	477.60	280.10	283.70	125.40	280.70	550.80	428.50	418.00	80.53
K(mg/L)	1.74	5.09	2.93	2.78	0.88	0.72	2.89	1.57	1.26	0.79	0.61	4.70	2.11	1.94	0.95
Na(mg/L)	13.56	66.90	39.58	41.17	16.23	81.88	349.90	236.20	244.30	91.53	352.90	832.00	529.10	525.30	121.10
Ca(mg/L)	35.61	189.30	96.65	70.48	60.68	ND	50.57	21.27	14.45	16.15	13.26	34.45	18.94	17.08	5.62
Mg(mg/L)	12.070	30.920	20.940	20.560	7.200	3.119	19.920	10.040	8.270	6.080	7.110	57.890	15.380	11.690	11.900
Fe(μg/L)	6.80	31.20	15.68	16.65	77.95	9.8	57.10	24.21	16.00	16.14	20.00	77.83	17.34	19.04	20.36
矿物饱和指数方解石	-0.37	0.35	-0.08	-0.24	0.29	-0.29	0.66	0.17	0.13	0.34	0.58	0.89	0.72	0.74	0.11
矿物饱和指数钠长石	-3.5	-1.45	-2.24	-2.06	0.69	-4.93	-1.42	-2.49	-2.43	0.94	-7.56	-4.72	-6.49	-6.59	0.73
矿物饱和指数钙长石	-4.63	-0.59	-2.41	-2.21	1.13	-5.33	-0.56	-1.41	-1.11	1.28	-5.7	-2.63	-4.19	-4.16	0.82
矿物饱和指数萤石	-2.25	-1.36	-1.84	-1.86	0.25	-1.73	0.34	-0.67	-0.52	0.77	0.09	0.86	0.51	0.49	0.19
矿物饱和指数岩盐	-8.2	-7.14	-7.66	-7.80	0.39	-7.90	-6.72	-7.42	-7.56	0.38	-7.46	-6.28	-6.90	-6.84	0.33
矿物饱和指数石膏	-2.42	-1.14	-1.80	-1.88	0.56	-1.72	-0.95	-1.15	-1.12	0.23	-1.13	-0.63	-0.92	-0.95	0.13
矿物饱和指数钾盐	-8.81	-7.65	-8.32	-8.35	0.43	-8.65	-7.39	-8.11	-8.10	0.33	-8.09	-6.71	-7.45	-7.35	0.38
矿物饱和指数绿泥石	-9.07	-4.50	-6.73	-6.8	1.24	-14.54	-5.13	-8.49	-8.00	2.61	-15.00	-7.65	-12.02	-12.08	1.64
矿物饱和指数高岭石	2.17	6.27	4.70	4.86	1.20	1.29	6.48	5.33	5.66	1.33	0.66	3.93	2.23	2.17	0.82
注：ND.未检出.

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表 3 Phreeqc反向地球化学模拟结果

Table 3. The result of inverse modeling of phreeqc along groundwater flow path

矿物相	化学式	转移量(mmol/L)
矿物相	化学式	Ⅰ区	Ⅱ区	Ⅲ区
方解石	CaCO₃	-1.480 0	2.500 0	1.380 0
钠长石	NaAlSi₃O₈	0.008 4	-3.350 0	-
钙长石	CaAl₂Si₂O₈	-0.004 2	-	-0.250 0
萤石	CaF₂	0.006 0	0.075 0	-
岩盐	NaCl	-1.20	4.76	8.94
石膏	CaSO₄:2H₂O	-1.48	1.81	-1.06
钾盐	KCl	0.017	-0.040	0.025
CO₂(g)	CO₂(g)	-1.68	-2.60	-
CaX₂	CaX₂	-0.43	-1.81	-
MgX₂	MgX₂	-0.42	-2.55	-0.19
NaX	NaX	1.69	8.73	0.37
绿泥石	Mg₅Al₂Si₃O₁₀(OH)₈	-	0.045	0.038
高岭石	Al₂Si₂O₅(OH)₄	-	3.40	0.21
注：正值表示迁入溶液(溶解)，负值表示迁出溶液(沉淀)，“-”表示无相关结果.

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