鄱阳湖流域赣江下游水化学特征及人类健康风险评价

doi:10.19657/j.geoscience.1000-8527.2022.018

摘要/Abstract

摘要：

人类活动对鄱阳湖赣江流域水质的影响受到广泛关注,厘清流域内污染水体对人类的健康风险状况有利于更好地保护和利用水资源。本研究于赣江下游采集39个地下水和16个地表水样,在分析其水化学特征和影响因素的基础上,对地下水水化学成分演变进行反向模拟,并对地下水水质以及潜在非致癌风险进行评价。结果表明,研究区地下水呈弱酸性-中性(pH=5.47~7.60),以HCO₃-Ca-Mg型水为主,部分为Cl-Ca-Mg型水,硅酸岩风化和矿物溶解-沉淀作用是水化学类型形成的主要控制因素;地表水呈中性-弱碱性(pH=6.94~8.19),主要为HCO₃-Cl-Ca-Na型水,其形成与硅酸岩风化、大气降水和人类活动有关。PHREEQC模拟计算结果表明,地下水中大部分矿物饱和指数(SI)为负数,其中岩盐的SI为-7.80~-9.53,指示该矿物溶解剧烈;白云石、石膏和方解石的SI分别为-1.72~-6.39、-1.65~-3.96、-0.51~-3.09,表明三种矿物呈溶解趋势。反向模拟结果显示,赣江干流地下水化学特征演变过程经历了Ca-蒙脱石、岩盐、白云石溶解和方解石沉淀,同时消耗CO₂;支流中命名为NCGW-3的路径表现为高岭石、方解石、玉髓和白云石溶解,石膏、Ca-蒙脱石、黑云母和斜长石沉淀,同时产生CO₂,可能与人为作用的干扰有关。其余支流地下水反向模拟结果与干流结果相似。熵权水质指数(EWQI)计算结果表明,干流地下水水质优于支流地下水,沿赣江受Mn、N $O 3 -$ 影响水质降低;地下水非致癌潜在风险主要为对婴儿存在严重风险,其次是儿童,对成年男性和成年女性风险相对较小,支流水质存在的潜在风险相较于干流更为显著。

关键词: 水文地球化学, PHREEQC, 反向模拟, 熵权水质指数, 人类健康风险评价

Abstract:

Anthropogenic impact on the water quality of Ganjiang River in the Poyang Lake basin has received wide attention. Understanding the health risks of polluted water is crucial for better protection and utilization of water resource. In this study, 39 groundwater and 16 surface water samples were collected from the downstream Ganjiang River to analyze for their geochemical characteristics and influencing factors. Inverse modelling was done to unravel the groundwater quality evolution. Groundwater quality and non-carcinogenic risk were further evaluated. Our results show that the local groundwater is weakly acidic to neutral (pH=5.47-7.60), dominated by HCO₃-Ca-Mg-type with minor Cl-Ca-Mg-type. Silicate weathering and mineral dissolution-precipitation impose the mainly control on the groundwater chemistry. Surface water is neutral to weakly-alkaline (pH=6.94-8.19) and mainly of HCO₃-Cl-Ca-Na-type, which is related to the weathering of silicate rocks, atmospheric precipitation and human activity. Hydrogeochemical calculations with PHREEQC show that the minerals have mostly negative halite saturation index (SI_Halite=-7.80 to -9.53), indicating that halite tends to dissolve. The low SI of dolomite (1.72 to -6.39), gypsum (-1.65 to -3.96) and calcite (-0.51 to -3.09) also indicate that these three minerals tend to be dissolved. The inverse modeling shows that groundwater evolution in the main stream has undergone dissolution of Ca-montmorillonite, halite, dolomite and calcite, and the consumption of CO₂. Results of groundwater inverse modeling in the tributaries are generally similar to those in the main stream, except for route NCGW-3, which indicates the dissolution of kaolinite, calcite, chalcopyrite, and colomite, and the precipitation of gypsum, Ca-montmorillonite, biotite and plagioclase, and the generation of CO₂. This may be attributed to human activities. Entropy-weighted water quality index (EWQI) calculation shows that groundwater quality in the main stream is better than that in the tributaries, and that the groundwater quality along the Ganjiang River is affected by Mn and N $O 3 -$ . The non-carcinogenic risk is the highest to infants, followed by children, but relatively low to adults. The risk is higher in the tributaries than in the main stream.

Key words: hydrochemistry, PHREEQC, inverse modeling, EWQI, health risk assessment

中图分类号:

P641.3
X143

吴通航, 刘海燕, 张卫民, 孙占学, 王振, 刘茂涵. 鄱阳湖流域赣江下游水化学特征及人类健康风险评价[J]. 现代地质, 2022, 36(02): 427-438.

WU Tonghang, LIU Haiyan, ZHANG Weimin, SUN Zhanxue, WANG Zhen, LIU Maohan. Hydrochemical Characteristics and Human Health Risk Assessment in Downstream Ganjiang River of the Poyang Lake Basin[J]. Geoscience, 2022, 36(02): 427-438.

图/表 14

图1 研究区水文地质图、采样点位置图(a)及剖面图(b)

Fig.1 Hydrogeological map of the study area, showing the sampling location (a), and profile map (b)

表1 EWQI等级分类

Table 1 Classification of EWQI

EWQI	等级	描述
≤50	1	优良
51~100	2	良好
101~150	3	中等
151~200	4	差
>200	5	极差

表2 HHRA模型相关参数

Table 2 Parameters of the HHRA model

人群分类	暴露参数					RfD_oral/(mg·kg^-1·a^-1)
人群分类	IR/ (L/d)	EF/ (d/a)	ED/a	BW/kg		N $O 3 -$		Mn
婴儿	0.65^*	365^*	0.5^*	6.94^*	1.6^**		0.14^*
儿童	1.50^*	365^*	6^*	25.9^*
成年男性	3.62^*	365^*	30^*	73.0^*
成年女性	2.66^*	365^*	30^*	64.0^*

表2 HHRA模型相关参数

Table 2 Parameters of the HHRA model

人群分类	暴露参数					RfD_oral/(mg·kg^-1·a^-1)
人群分类	IR/ (L/d)	EF/ (d/a)	ED/a	BW/kg		N $O 3 -$		Mn
婴儿	0.65^*	365^*	0.5^*	6.94^*	1.6^**		0.14^*
儿童	1.50^*	365^*	6^*	25.9^*
成年男性	3.62^*	365^*	30^*	73.0^*
成年女性	2.66^*	365^*	30^*	64.0^*

表3 研究区水化学特征参数

Table 3 Hydrogeochemical parameters for the water samples

区域	统计参数	pH	ORP/ mV	EC/ (μV/cm)	TDS/ (mg/L)	Cl^-/ (mg/L)	S $O 4 2 -$ / (mg/L)	HC $O 3 -$ / (mg/L)	Ca²⁺/ (mg/L)	K⁺/ (mg/L)	Mg²⁺/ (mg/L)	Na⁺/ (mg/L)	N $O 3 -$ / (mg/L)	Mn/ (μg/L)
干流地下水	最小值	5.47	-99.50	126.40	63.20	1.72	0.16	8.00	8.51	0	2.90	3.45	0	2.17
	最大值	7.00	302.00	1 632.00	880.00	76.74	64.11	376.00	89.58	78.33	27.13	39.98	91.66	6 150.00
	平均值	6.46	112.87	438.83	225.61	31.07	18.73	106.83	28.09	13.79	9.75	14.62	27.48	861.24
	标准偏差	0.40	99.73	307.09	166.34	20.12	17.65	77.69	19.15	17.40	5.27	8.34	29.86	1 636.35
	指导值	6.5~8.5^*	—	2 500^**	1 000^*	250^*	250^*	—	75^**	200^**	50^**	200^**	50^**	100^*
支流地下水	最小值	5.66	106.50	47.20	23.60	2.23	3.58	13.59	4.70	1.00	2.10	3.11	5.24	1.80
	最大值	7.60	232.00	731.00	365.50	86.06	111.91	108.74	57.42	62.93	14.20	31.58	158.15	2 191.00
	平均值	6.68	174.12	247.21	123.60	19.63	26.07	44.48	24.36	11.19	5.12	9.82	39.73	303.41
	标准偏差	0.61	39.88	209.98	104.99	24.45	31.31	36.01	18.76	17.76	3.31	8.51	44.52	642.45
	指导值	6.5~8.5^*	—	2 500^**	1 000^*	250^*	250^*	—	75^**	200^**	50^**	200^**	50^**	100^*
地表水	最小值	6.94	-17.40	173.90	86.95	11.19	6.94	40.78	17.22	3.25	3.09	9.50	1.14	3.63
	最大值	8.19	220.00	304.00	152.00	31.36	30.91	81.56	25.13	12.02	5.00	20.09	7.22	107.00
	平均值	7.52	135.51	216.59	108.30	21.00	17.41	61.17	20.01	5.85	3.52	13.02	4.02	35.63
	标准偏差	0.41	57.33	51.89	25.94	6.52	8.32	9.93	3.16	2.91	0.58	4.07	2.36	31.54

表3 研究区水化学特征参数

Table 3 Hydrogeochemical parameters for the water samples

区域	统计参数	pH	ORP/ mV	EC/ (μV/cm)	TDS/ (mg/L)	Cl^-/ (mg/L)	S $O 4 2 -$ / (mg/L)	HC $O 3 -$ / (mg/L)	Ca²⁺/ (mg/L)	K⁺/ (mg/L)	Mg²⁺/ (mg/L)	Na⁺/ (mg/L)	N $O 3 -$ / (mg/L)	Mn/ (μg/L)
干流地下水	最小值	5.47	-99.50	126.40	63.20	1.72	0.16	8.00	8.51	0	2.90	3.45	0	2.17
	最大值	7.00	302.00	1 632.00	880.00	76.74	64.11	376.00	89.58	78.33	27.13	39.98	91.66	6 150.00
	平均值	6.46	112.87	438.83	225.61	31.07	18.73	106.83	28.09	13.79	9.75	14.62	27.48	861.24
	标准偏差	0.40	99.73	307.09	166.34	20.12	17.65	77.69	19.15	17.40	5.27	8.34	29.86	1 636.35
	指导值	6.5~8.5^*	—	2 500^**	1 000^*	250^*	250^*	—	75^**	200^**	50^**	200^**	50^**	100^*
支流地下水	最小值	5.66	106.50	47.20	23.60	2.23	3.58	13.59	4.70	1.00	2.10	3.11	5.24	1.80
	最大值	7.60	232.00	731.00	365.50	86.06	111.91	108.74	57.42	62.93	14.20	31.58	158.15	2 191.00
	平均值	6.68	174.12	247.21	123.60	19.63	26.07	44.48	24.36	11.19	5.12	9.82	39.73	303.41
	标准偏差	0.61	39.88	209.98	104.99	24.45	31.31	36.01	18.76	17.76	3.31	8.51	44.52	642.45
	指导值	6.5~8.5^*	—	2 500^**	1 000^*	250^*	250^*	—	75^**	200^**	50^**	200^**	50^**	100^*
地表水	最小值	6.94	-17.40	173.90	86.95	11.19	6.94	40.78	17.22	3.25	3.09	9.50	1.14	3.63
	最大值	8.19	220.00	304.00	152.00	31.36	30.91	81.56	25.13	12.02	5.00	20.09	7.22	107.00
	平均值	7.52	135.51	216.59	108.30	21.00	17.41	61.17	20.01	5.85	3.52	13.02	4.02	35.63
	标准偏差	0.41	57.33	51.89	25.94	6.52	8.32	9.93	3.16	2.91	0.58	4.07	2.36	31.54

图2 研究区采样点水样Piper三线图(单位: %)

Fig.2 Piper plots of water samples from the study area(unit: %)

图3 研究区采样点水样Gibbs图

Fig.3 Gibbs diagrams of water samples from the study area

图4 研究区水样Ca2+/Na+和HC03-/Na+关系

Fig.4 Bivariate molar ratio plot of Ca2+/Na+ vs. HC03-/Na+ of water samples from the study area

图5 地下水矿物饱和指数

Fig.5 Mineral SI for the groundwater samples

表4 反向模拟数据点

Table 4 Data points selected for inverse modelling

反向模拟路径	路径起点 /终点	pH	Cl^-/ (mg/L)	S $O 4 2 -$ / (mg/L)	N $O 3 -$ / (mg/L)	HC $O 3 -$ / (mg/L)	Ca²⁺/ (mg/L)	K⁺/ (mg/L)	Mg²⁺/ (mg/L)	Na⁺/ (mg/L)
NCGW-1	gj-3	6.83	2.23	18.90	5.24	54.37	15.68	2.97	3.60	4.42
NCGW-1	gj-12	5.66	86.06	35.29	158.15	13.59	39.94	62.93	14.20	31.58
NCGW-2	gj-21	6.85	203.89	28.85	16.76	6.41	10.04	203.89	28.85	16.76
NCGW-2	gj-28	6.80	40.78	9.99	7.74	6.38	13.03	40.78	9.99	7.74
NCGW-3	gj-54	6.05	20.36	54.49	70.17	66.00	42.05	13.75	9.92	9.26
NCGW-3	gj-46	6.38	20.92	4.54	8.71	104.00	17.81	0	8.56	6.75
NCGW-4	gj-52	6.60	28.77	22.88	1.72	142.00	48.37	12.51	7.36	9.72
NCGW-4	gj-48	6.31	24.97	12.26	4.94	66.00	17.52	9.47	9.48	7.29

表4 反向模拟数据点

Table 4 Data points selected for inverse modelling

反向模拟路径	路径起点 /终点	pH	Cl^-/ (mg/L)	S $O 4 2 -$ / (mg/L)	N $O 3 -$ / (mg/L)	HC $O 3 -$ / (mg/L)	Ca²⁺/ (mg/L)	K⁺/ (mg/L)	Mg²⁺/ (mg/L)	Na⁺/ (mg/L)
NCGW-1	gj-3	6.83	2.23	18.90	5.24	54.37	15.68	2.97	3.60	4.42
NCGW-1	gj-12	5.66	86.06	35.29	158.15	13.59	39.94	62.93	14.20	31.58
NCGW-2	gj-21	6.85	203.89	28.85	16.76	6.41	10.04	203.89	28.85	16.76
NCGW-2	gj-28	6.80	40.78	9.99	7.74	6.38	13.03	40.78	9.99	7.74
NCGW-3	gj-54	6.05	20.36	54.49	70.17	66.00	42.05	13.75	9.92	9.26
NCGW-3	gj-46	6.38	20.92	4.54	8.71	104.00	17.81	0	8.56	6.75
NCGW-4	gj-52	6.60	28.77	22.88	1.72	142.00	48.37	12.51	7.36	9.72
NCGW-4	gj-48	6.31	24.97	12.26	4.94	66.00	17.52	9.47	9.48	7.29

表5 不同路径的相摩尔转移量(mol/L)

Table 5 Molar transfer for phases in different routes (mol/L)

反向模拟路径	岩盐	石膏	高岭石	Ca-蒙脱石	CO₂(气)	方解石	玉髓	黑云母	斜长石	白云石
NCGW-1	5.31E-04	-5.57E-03	-1.42E+03	1.22E+03	2.01E+02	-2.01E+02	-1.63E+03	-3.46E-03	-8.00E-03	6.50E-03
NCGW-2	-1.81E-02	-7.12E-03	-9.85E+02	8.45E+02	1.39E+02	-1.40E+02	-1.13E+03	-5.48E-02	1.51E-02	1.60E-01
NCGW-3	5.21E-04	-2.15E-05	4.27E+01	-3.67E+01	-6.05E+00	6.05E+00	4.92E+01	-5.44E-04	-4.45E-04	2.49E-03
NCGW-4	-4.71E-04	-2.07E-04	-1.97E+01	1.69E+01	2.79E+00	-2.80E+00	-2.27E+01	-2.08E-04	3.12E-04	5.87E-04

图6 地下水EWQI散点图

Fig.6 Groundwater EWQI scatter plots

图7 研究区干流地下水危险系数箱线图

Fig.7 Box line diagrams of risk factor for the mainstream groundwater of the study area

图8 研究区支流地下水危险系数箱线图

Fig.8 Box line diagrams of risk factor for the tributaries groundwater of the study area

图9 研究区地下水潜在非致癌风险状况

Fig.9 Potential non-carcinogenic risk status of groundwater from the study area

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