海拉尔盆地水环境中砷和铀的分布特征及风险评价

doi:10.19657/j.geoscience.1000-8527.2022.020

现代地质 ›› 2023, Vol. 37 ›› Issue (04): 933-942.DOI: 10.19657/j.geoscience.1000-8527.2022.020

海拉尔盆地水环境中砷和铀的分布特征及风险评价

刘圣锋¹(), 高柏¹^,²(), 易玲³, 方正¹, 史天成¹, 丁燕¹

1.东华理工大学水资源与环境工程学院,江西南昌 330013
2.东华理工大学核资源与环境国家重点实验室,江西南昌 330013
3.江西省地质环境监测所,江西南昌 330012

收稿日期:2022-01-18 修回日期:2022-04-17 出版日期:2023-08-10 发布日期:2023-09-02
通讯作者: 高柏,男,教授,博士生导师,1964年出生,地质资源与地质工程专业,主要从事地下水污染与修复研究。Email:gaobai@ecit.cn。
作者简介:高柏,男,教授,博士生导师,1964年出生,地质资源与地质工程专业,主要从事地下水污染与修复研究。Email:gaobai@ecit.cn。
刘圣锋,男,硕士研究生,1996年出生,水利工程专业,主要从事地下水污染与治理研究。Email:1372729482@qq.com。
基金资助:
国家自然科学基金项目(42272301);江西省研究生创新基金项目(YC2021-S626);江西省重点研发计划项目(2018ACG70023)

Arsenic-Uranium Distribution Characteristics and Risk Assessment in the Aquatic Environment of Hailar Basin

LIU Shengfeng¹(), GAO Bai¹^,²(), YI Ling³, FANG Zheng¹, SHI Tiancheng¹, DING Yan¹

1. School of Water Resources & Environmental Engineering, East China University of Technology, Nanchang, Jiangxi 330013, China
2. State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang, Jiangxi 330013, China
3. Jiangxi Provincial Geological Environment Monitoring Institute, Nanchang, Jiangxi 330012, China

Received:2022-01-18 Revised:2022-04-17 Online:2023-08-10 Published:2023-09-02

摘要/Abstract

摘要：

海拉尔盆地位于干旱-半干旱地区,降水量少,蒸发量大,水资源相对匮乏。另外,由于该盆地存在丰富的砂岩型铀矿床,矿石中的As和U常常通过岩石风化、阳离子交换和降水淋滤等作用进入水环境中,其水资源污染状况堪忧。基于此,本研究在野外采样数据的基础上,分析海拉尔盆地地下水及地表水水化学特征和影响因素,利用PHREEQC软件对As和U的存在形态进行模拟,并对As和U共污染现象进行特征分析及风险评价。结果表明,海拉尔盆地水环境中As和U的浓度大部分超出了世界卫生组织(WHO)的标准限值。在贝尔湖坳陷—嵯岗隆起地带水环境中As浓度较高,嵯岗隆起靠近呼伦湖附近U的浓度较高。经美国环境保护局(US EPA)健康风险评价模型计算,不同人群的平均非致癌总风险HI_total均超过了可接受水平(HI_total<1),As的致癌风险平均值也均超过了可接受范围水平(1×10^-6),非致癌总风险和致癌风险儿童>成年女性>成年男性。PHREEQC模拟结果显示,水环境中As主要以As(V)形式存在,大部分采样点以 $HAsO 4 2 -$ 、H₂ $AsO 4 -$ 等形态为主,U以VI价的UO₂(CO₃) $3 4 -$ 、UO₂(CO₃) $2 2 -$ 为主。As的化学价态易受到pH和Eh值影响,pH值减小以及在相对还原条件下,容易形成毒性更强的As(III)。U的化学价态没有明显受到pH和Eh值影响,但改变pH和Eh值也会形成沥青铀矿等固体沉淀,可能会引发结石等相关疾病。

关键词: 砷, 铀, 分布特征, 赋存形态, 健康风险, 海拉尔盆地

Abstract:

The Hailar Basin is located in an arid to semi-arid region, and its water resource has received widespread attention. Studying the hydrogeochemical characteristics of the local water environment and health risk assessment is conducive to better protection and utilization of water resource. Based on field sampling data, we analyzed its hydrochemical characteristics and influence factors, used the PHREEQC software to simulate the As-U occurrence, and conducted characteristic analysis and risk assessment of As-U co-pollution phenomena. The results show that the As-U concentrations in the local water environment mostly exceed the World Health Organization (WHO) standard limits. The As concentration in the water environment in the Beier Lake Depression-Cuogang Uplift is higher, and the U concentration in the Cuogang Uplift near Hulun Lake is higher. Calculated by the US EPA health risk assessment model, the average non-carcinogenic total risk HI_total of different populations all exceed the acceptable level (HI_total <1), and the average carcinogenic risk of As also exceeds the acceptable level (1×10^-6). The total non-carcinogenic risk and carcinogenic risk: children>female adult>male adult. The PHREEQC simulation results show that As in the water environment mainly exists in the form of As(V), and most of the sampling spots are dominated by $HAsO 4 2 -$ and H₂ $AsO 4 -$ . Uranium occurs mainly in the form of U(VI): UO₂(CO₃) $3 4 -$ and UO₂(CO₃) $2 2 -$ . The chemical valence of As is readily affec-ted by the pH and Eh values. The pH decrease and the more toxic As(III) are likely formed under relatively reducing conditions. The chemical valence of U is not strongly affected by the pH and Eh values, but changing which would also form solid deposits such as bituminous uranium ore, which may cause stones and other related diseases.

Key words: arsenic, uranium, distribution characteristics, occurrence mode, health risk, Hailar basin

中图分类号:

P641.12

刘圣锋, 高柏, 易玲, 方正, 史天成, 丁燕. 海拉尔盆地水环境中砷和铀的分布特征及风险评价[J]. 现代地质, 2023, 37(04): 933-942.

LIU Shengfeng, GAO Bai, YI Ling, FANG Zheng, SHI Tiancheng, DING Yan. Arsenic-Uranium Distribution Characteristics and Risk Assessment in the Aquatic Environment of Hailar Basin[J]. Geoscience, 2023, 37(04): 933-942.

图/表 9

图1 采样点分布

Fig.1 Distribution of sampling locations

表1 海拉尔盆地水质指标特征

Table 1 Characteristics of water quality indicators in the Hailar Basin

水样类型	项目	pH	TDS	Eh	K⁺	Na⁺	Ca²⁺	Mg²⁺	Cl^-	$SO 4 2 -$	$NO 3 -$	$HCO 3 -$	Fe²⁺	Fe³⁺	As	U
地表水	最小值	8.16	255.00	163.00	4.57	38.70	23.94	17.49	13.60	4.29	0.00	345.43	0.078	0.086	0.024	0.018
	最大值	9.88	1080.00	238.00	15.06	251.85	38.45	64.65	97.97	32.68	0.32	673.94	0.160	0.743	0.102	0.135
	平均值	8.94	648.75	191.25	10.67	166.15	29.47	39.02	59.08	17.93	0.08	467.51	0.112	0.344	0.060	0.072
	标准差	0.66	351.45	29.34	3.87	88.33	5.85	17.05	31.97	13.52	0.14	123.68	0.030	0.244	0.033	0.044
	变异系数	0.07	0.54	0.15	0.36	0.53	0.20	0.44	0.54	0.75	1.73	0.26	0.272	0.710	0.542	0.609
地下水	最小值	7.12	244.00	-133.00	0.67	12.87	5.79	5.23	4.16	4.17	0.00	90.04	0.029	0.085	0.005	0.017
	最大值	8.63	3690.00	329.00	49.17	625.79	123.11	164.03	909.33	417.82	32.81	803.11	0.131	4.477	0.123	0.257
	平均值	7.77	1195.44	188.52	7.77	5.28	240.83	49.85	224.41	97.44	7.59	405.36	0.052	0.411	0.036	0.075
	标准差	0.34	819.06	100.86	7.98	175.62	26.62	28.78	230.55	94.47	6.96	160.13	0.023	0.854	0.025	0.048
	变异系数	0.04	0.69	0.54	1.51	0.73	0.53	0.68	1.03	0.97	0.92	0.40	0.436	2.080	0.689	0.637

表1 海拉尔盆地水质指标特征

Table 1 Characteristics of water quality indicators in the Hailar Basin

水样类型	项目	pH	TDS	Eh	K⁺	Na⁺	Ca²⁺	Mg²⁺	Cl^-	$SO 4 2 -$	$NO 3 -$	$HCO 3 -$	Fe²⁺	Fe³⁺	As	U
地表水	最小值	8.16	255.00	163.00	4.57	38.70	23.94	17.49	13.60	4.29	0.00	345.43	0.078	0.086	0.024	0.018
	最大值	9.88	1080.00	238.00	15.06	251.85	38.45	64.65	97.97	32.68	0.32	673.94	0.160	0.743	0.102	0.135
	平均值	8.94	648.75	191.25	10.67	166.15	29.47	39.02	59.08	17.93	0.08	467.51	0.112	0.344	0.060	0.072
	标准差	0.66	351.45	29.34	3.87	88.33	5.85	17.05	31.97	13.52	0.14	123.68	0.030	0.244	0.033	0.044
	变异系数	0.07	0.54	0.15	0.36	0.53	0.20	0.44	0.54	0.75	1.73	0.26	0.272	0.710	0.542	0.609
地下水	最小值	7.12	244.00	-133.00	0.67	12.87	5.79	5.23	4.16	4.17	0.00	90.04	0.029	0.085	0.005	0.017
	最大值	8.63	3690.00	329.00	49.17	625.79	123.11	164.03	909.33	417.82	32.81	803.11	0.131	4.477	0.123	0.257
	平均值	7.77	1195.44	188.52	7.77	5.28	240.83	49.85	224.41	97.44	7.59	405.36	0.052	0.411	0.036	0.075
	标准差	0.34	819.06	100.86	7.98	175.62	26.62	28.78	230.55	94.47	6.96	160.13	0.023	0.854	0.025	0.048
	变异系数	0.04	0.69	0.54	1.51	0.73	0.53	0.68	1.03	0.97	0.92	0.40	0.436	2.080	0.689	0.637

图2 研究区水样Piper三线图

Fig.2 Piper diagram for water samples form the study area

表2 地表水采样点中砷和铀的含量

Table 2 Arsenic and uranium contents in surface water sampling spots

地表水采样编号	采样点经度	采样点纬度	砷(mg/L)	铀(mg/L)
H1	118°47'05″	48°45'09″	0.082	0.018
H2	117°43'12″	47°58'09″	0.024	0.048
H3	118°11'26″	48°13'12″	0.033	0.087
H4	118°09'28″	48°23'28″	0.102	0.135

图3 地下水中砷和铀含量

Fig.3 Contour map of arsenic-uranium contents in groundwater

图4 研究区水样Gibbs图

Fig.4 Gibbs diagram for water samples from the study area

图5 不同人群健康风险评价 (a)非致癌风险;(b)致癌风险

Fig.5 Health risk assessment of different populations

图6 研究区水样中As和U主要存在形态

Fig.6 Main occurrence forms of As and U in water samples from the study area

图7 不同pH和Eh值下As和U的赋存形态变化[37-38]

Fig.7 Relationship between As and U under different pH and Eh values [37-38]

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海拉尔盆地水环境中砷和铀的分布特征及风险评价

Arsenic-Uranium Distribution Characteristics and Risk Assessment in the Aquatic Environment of Hailar Basin

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