华北平原典型山前冲洪积扇高硝态氮地下水分布特征及健康风险评价

doi:10.13745/j.esf.sf.2023.2.53

地学前缘 ›› 2023, Vol. 30 ›› Issue (4): 485-503.DOI: 10.13745/j.esf.sf.2023.2.53

华北平原典型山前冲洪积扇高硝态氮地下水分布特征及健康风险评价

张广禄¹^,²(), 刘海燕¹^,²^,^*(), 郭华明³, 孙占学¹^,², 王振¹^,², 吴通航¹^,²

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:2022-06-01 修回日期:2022-12-23 出版日期:2023-07-25 发布日期:2023-07-07
通讯作者: *刘海燕(1988—),男,博士,讲师,主要从事水文地球化学研究工作。E⁃mail: hy_liu@ecut.edu.cn
作者简介:张广禄(1998-),男,硕士研究生,主要从事水文地球化学研究。E-mail: 972591540@qq.com
基金资助:
江西省自然科学基金项目(20202BABL211018);国家自然科学基金项目(41902243);国家自然科学基金项目(42262029)

Occurrences and health risks of high-nitrate groundwater in typical piedmont areas of the North China Plain

ZHANG Guanglu¹^,²(), LIU Haiyan¹^,²^,^*(), GUO Huaming³, SUN Zhanxue¹^,², WANG Zhen¹^,², WU Tonghang¹^,²

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:2022-06-01 Revised:2022-12-23 Online:2023-07-25 Published:2023-07-07

摘要/Abstract

摘要：

地下水硝态氮污染受到世界的广泛关注,但是,高集约农业生产的山前冲洪积扇地下水中高硝态氮分布特征及其对不同人群的健康危害尚未完全清楚。本研究于华北平原北京和石家庄地区两组冲洪积扇采集了144件地下水样,在研究地下水化学成分形成控制因素的基础上,探究地下水中高硝态氮的分布规律与成因机制以及健康风险。结果表明地下水为中性至弱碱性。84%地下水样品的硝态氮浓度超出我国饮用水标准值10 mg/L,北京地区地下水硝态氮平均浓度高于石家庄地区。两地区总体浅层地下水硝态氮浓度高于深层地下水,西南部地区地下水硝态氮高于东部和北部地区。高硝态氮地下水水化学类型以HCO₃-Ca-Mg型为主。地下水化学形成作用主要受矿物溶解、岩石风化和蒸发结晶的影响。离子比例系数和主成分分析(PCA)表明,农业活动、离子交换和硝化作用是高硝态氮地下水形成的主要原因。深层地下水水质优良且熵权水质指数(EWQI)多处于1或2等级,优于浅层地下水。人类健康风险评价(HHRA)模型对4类人群(婴儿、儿童、成年男性、成年女性)风险计算结果显示:地下水硝态氮的潜在非致癌风险对婴儿表现严重,浅层地下水潜在非致癌风险都要高于深层地下水,石家庄地区地下水潜在非致癌风险低于北京地区。平面上,北京地区地下水硝态氮对4类人群均存在潜在风险,高风险区域主要分布在北京西南部和中部,东部风险相对较低。石家庄地区地下水硝态氮潜在风险整体表现为西高东低,东部大部分区域地下水适宜全部人群饮用。因此,控制浅层地下水硝态氮的输入、根据不同人群差别取水、对婴儿群体多提供深层地下水源是保障居民饮水安全的关键。

关键词: 氮循环, 水岩作用, 地下水污染, 华北平原, 人类健康风险评价

Abstract:

Nitrate pollution in groundwater is a global concern, yet the distribution characteristics of high-nitrate groundwater and its health risks to different populations in the agricultural intensive piedmont alluvial fans are not fully understood. In this study, we carried out comprehensive hydrogeochemical analysis on 144 groundwater samples collected from two sets of piedmont aquifers (Beijing and Shijiazhuang areas) in the North China Plain to determine the distribution pattern, formation mechanism, and health risks of high-nitrate groundwater in the region. The regional groundwater was neutral to slightly alkaline, and 84% of the samples had nitrate concentrations exceeding the national standard (10 mg/L) for drinking water. The average nitrate concentration in groundwater was higher in Beijing than in Shijiazhuang areas, and in both areas higher in shallow than in deep aquifers. Planarly, high-nitrate groundwater was more commonly distributed in the southwestern region as compared to the eastern and northern regions. High-nitrate groundwater was mainly characterized by HCO₃-Ca-Mg hydrochemical facies, controlled mainly by mineral dissolution, rock weathering, and evaporative crystallization, according to ion ratio and principal component analyses. Agricultural activities, ion exchange, and nitrification were the main causes of nitrate enrichment in groundwater. Water quality of deep groundwater was better compared to shallow groundwater, with EWQI values mostly between 1 and 2. According to health risks assessments of four population groups (infants, children, women, and men) using HHRA model, the potential non-carcinogenic risk of high-nitrate groundwater was high for infants, and shallow groundwater posed a greater health risk in both areas. Overall, the potential non-carcinogenic risks were lower in Shijiazhuang than in Beijing where high-nitrate groundwater posed a health risk to all populations. In Beijing, the high risk areas were mainly located in the southwest and central part, and the east was at relative low risk. In Shijiazhuang, the potential health risk was high in the west and low in the east, and most of the groundwater in the east was suitable for drinking by all populations. We concluded, therefore, that controlling nitrate input from shallow groundwater, selecting drinking water sources according to population groups, and providing deep groundwater to infants were crucial for ensuring safe drinking water for local residents.

Key words: nitrogen cycle, water-rock interaction, groundwater pollution, North China Plain, human health risk assessment

中图分类号:

张广禄, 刘海燕, 郭华明, 孙占学, 王振, 吴通航. 华北平原典型山前冲洪积扇高硝态氮地下水分布特征及健康风险评价[J]. 地学前缘, 2023, 30(4): 485-503.

ZHANG Guanglu, LIU Haiyan, GUO Huaming, SUN Zhanxue, WANG Zhen, WU Tonghang. Occurrences and health risks of high-nitrate groundwater in typical piedmont areas of the North China Plain[J]. Earth Science Frontiers, 2023, 30(4): 485-503.

图/表 18

图1 研究区和采样点分布图

Fig.1 Map of the study area and sampling locations

图2 研究区水文地质剖面图(AA':BJ区;BB':SJZ区)

Fig.2 Hydrogeological cross-sections along AA' line in Beijing (BJ) and BB' line in Shijiazhuang (SJZ) areas (profile locations see Fig.1)

表1 HHRA模型相关参数

Table 1 HHRA model parameters

人群分类	暴露参数
人群分类	IR/(L·d^-1)	EF/(d·a^-1)	ED/a	BW/kg
婴儿	0.65	365	0.5	6.94
儿童	21.5	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 研究区水化学参数表

Table 2 Hydrochemical parameters for regional groundwater

图3 研究区地下水硝态氮浓度分布图

Fig.3 Distribution of nitrate concentrations in regional groundwater

图4 研究区地下水样piper三线图

Fig.4 Piper plots for groundwater samples in the study area

图5 硝态氮浓度垂向分布图

Fig.5 Vertical distribution of nitrate concentrations

图6 硝态氮含量平面分布图 a-BJ区;b-SJZ区。

Fig.6 Spatial distribution of nitrate concentrations in (a) BJ and (b) SJZ areas

表3 主成分旋转变量表

Table 3 Rotated principal components

初始变量	各主成分中变量的载荷量
初始变量	PC1	PC2	PC3
pH	-0.73	0.12	-0.37
ORP	-0.04	0.26	0.67
组分浓度
TDS	0.92	0.32	0.17
Cl^-	0.75	0.38	0.38
SO₄^2-	0.77	0.37	-0.26
HCO₃^-	0.74	0.15	0.41
Ca²⁺	0.96	-0.06	-0.03
K⁺	0.04	0.86	0.00
Mg²⁺	0.76	0.34	0.22
Na⁺	0.44	0.71	0.26
NO₃^-	0.82	0.11	0.04
Mn	0.18	-0.07	0.61
特征值	5.47	1.86	1.49
方差贡献率/%	45.6	15.5	12.5
累积贡献率/%	45.6	61.1	73.6

图7 地下水各水化学参数之间的相关矩阵图

Fig.7 Correlation matrix for hydrochemical parameters for groundwater

图8 地下水相关离子散点图图中坐标轴上所示离子浓度均为物质的量浓度。a-Na+与Cl-;b-Ca2+与SO42-;c-(Ca2++Mg2+)与HCO3-;d-(Ca2++Mg2+)与(HCO3-+SO42-);e-CAI-I与CAI-II;f-(Na++K+-Cl-)与(Ca2++Mg2+-HCO3-SO42-)。

Fig.8 Correlation plots for ionic species in regional groundwater

图9 研究区地下水样Gibbs图 a图中的Na+/(Na++Ca2+)和b图中的Cl-/(Cl-+HCO3-)均为质量分数比。

Fig.9 Gibbs diagrams identifying the main processes controlling high-nitrate groundwater in the study area

图10 Ca2+/Na+与Mg2+/Na+(a)和HCO3-/Na+(b)的关系图图中比值均为摩尔分数比。

Fig.10 Bivariate plots of mole fraction ratios Ca2+/Na+ vs. Mg2+/Na+ (a) and HCO3-/Na+ (b)

图11 (Ca2++Mg2++Na++K+-Cl-SO42-)与HCO3-浓度散点图(a)和SO42-/Ca2+与NO3-/Ca2+比值散点关系图(b) 图中坐标轴上所示离子浓度均为物质的量浓度,比值为摩尔分数比。

Fig.11 Scatter plots of (Ca2++Mg2++Na++K+-Cl--SO42-) vs. HCO3- (a) and SO42-/Ca2+ vs. NO3-/Ca2+ (mole fraction ratios) (b)

图12 不同硝态氮浓度地下水水样的pH与ORP散点图(a)和硝态氮浓度与EWQI散点图(b)

Fig.12 Scatter plots of NO3- vs. ORP (a), and NO3- vs. EWQI (b)

图13 地下水硝态氮危险系数箱线图 a-BJ区;b-SJZ区。

Fig.13 Box plots comparing nitrate hazard quotient ( H Q N O 3 - ) values in deep and shallow groundwater for different population groups in BJ (a) and SJZ (b) areas

图14 BJ区硝态氮HQ值的空间分布图 a-婴儿;b-儿童;c-成年男性;d-成年女性。

Fig.14 Spatial distributions of H Q N O 3 - values for different population groups in BJ area. (a) Infants; (b) Children; (c) Women; (d) Men.

图15 SJZ区硝态氮HQ值的空间分布图 a-婴儿;b-儿童;c-成年男性;d-成年女性。

Fig.15 Spatial distributions of H Q N O 3 - values for different population groups in SJZ area. (a) Infants; (b) Children; (c) Women; (d) Men.

参考文献 59

[1]	ZHANG Y H, DAI Y S, WANG Y, et al. Hydrochemistry, quality and potential health risk appraisal of nitrate enriched groundwater in the Nanchong area, southwestern China[J]. Science of the Total Environment, 2021, 784: 147186. DOI URL
[2]	张婧, 马贵宏, 高雅, 等. 华北山前平原典型井灌区地下水水位变化影响因素分析[J]. 河海大学学报(自然科学版), 2022, 50(1): 21-28, 84.
[3]	DÖLL P, HOFFMANN-DOBREV H, PORTMANN F T, et al. Impact of water withdrawals from groundwater and surface water on continental water storage variations[J]. Journal of Geodynamics, 2012, 59/60: 143-156. DOI URL
[4]	万长园. 华北平原典型区地下水三氮时空分布与运移数值模拟研究[D]. 阜新: 辽宁工程技术大学, 2014.
[5]	张兆吉, 费宇红, 郭春艳, 等. 华北平原区域地下水污染评价[J]. 吉林大学学报(地球科学版), 2012, 42(5): 1456-1461.
[6]	FENECH C, ROCK L, NOLAN K, et al. The potential for a suite of isotope and chemical markers to differentiate sources of nitrate contamination: a review[J]. Water Research, 2012, 46(7): 2023-2041. DOI PMID
[7]	刘琰, 乔肖翠, 江秋枫, 等. 滹沱河冲洪积扇地下水硝酸盐含量的空间分布特征及影响因素[J]. 农业环境科学学报, 2016, 35(5): 947-954.
[8]	SMITH K A, ANTHONY S G, HENDERSON D, et al. Critical drainage and nitrate leaching losses from manures applied to freely draining soils in Great Britain[J]. Soil Use and Management, 2003, 19(4): 312-320. DOI URL
[9]	BABIKER I S, MOHAMED M A A, TERAO H, et al. Assessment of groundwater contamination by nitrate leaching from intensive vegetable cultivation using geographical information system[J]. Environment International, 2004, 29(8): 1009-1017. DOI PMID
[10]	陈淑峰, 李帷, 胡克林, 等. 基于GIS的华北高产粮区地下水硝态氮含量时空变异特征[J]. 环境科学, 2009, 30(12): 3541-3547.
[11]	ZHANG W L, TIAN Z X, ZHANG N, et al. Nitrate pollution of groundwater in northern China[J]. Agriculture, Ecosystems and Environment, 1996, 59(3): 223-231. DOI URL
[12]	WHO World Health Organization. Guideline for drinking water quality[S]. 4th ed. Geneva: World Health Organization, 2011.
[13]	叶浩, 刘长礼, 姜建梅, 等. 滹沱河石家庄段地下水污染风险评价[J]. 地质通报, 2008, 27(7): 1065-1070.
[14]	贺国平, 刘培斌, 慕星, 等. 永定河冲洪积扇地下水中硝酸盐来源的同位素识别[J]. 水利学报, 2016, 47(4): 582-588.
[15]	国家市场监督管理总局, 国家标准化管理委员会. 生活饮用水卫生标准: GB 5749-2022[S]. 北京: 中国标准出版社, 2022.
[16]	JOHNSON P T J, TOWNSEND A R, CLEVELAND C C, et al. Linking environmental nutrient enrichment and disease emergence in humans and wildlife[J]. Ecological Applications, 2010, 20(1): 16-29. DOI URL
[17]	DAVIDSON E A, DAVID M B, GALLOWAY J N, et al. Excess nitrogen in the U.S. environment: trends, risks, and solutions[J]. Issues in Ecology, 2012, 15: 1-16.
[18]	陈建耀, 王亚, 张洪波, 等. 地下水硝酸盐污染研究综述[J]. 地理科学进展, 2006, 25(1): 34-44.
[19]	陈耀宁, 智国铮, 袁兴中, 等. 基于三角随机模拟和ArcGIS的河流水环境健康风险评价模型[J]. 环境工程学报, 2016, 10(4): 1799-1806.
[20]	章艳红, 唐玉红, 陈俊华, 等. 萍水河地表水重金属污染特征及健康风险评价[J]. 有色金属(冶炼部分), 2021(7): 116-125.
[21]	WANG H L, LU K Y, SHEN C Y, et al. Human health risk assessment of groundwater nitrate at a two geomorphic units transition zone in northern China[J]. Journal of Environmental Sciences, 2021, 110(12): 38-47. DOI URL
[22]	LI D F, ZHAI Y Z, LEI Y, et al. Spatiotemporal evolution of groundwater nitrate nitrogen levels and potential human health risks in the Songnen Plain, Northeast China[J]. Ecotoxicology and Environmental Safety, 2021, 208: 111524. DOI URL
[23]	PANDA B, CHIDAMBARAM S, SNOW D, et al. Source apportionment and health risk assessment of nitrate in foothill aquifers of Western Ghats, South India[J]. Ecotoxicology and Environmental Safety, 2022, 229: 113075. DOI URL
[24]	钱永, 张兆吉, 费宇红, 等. 华北平原浅层地下水可持续利用潜力分析[J]. 中国生态农业学报, 2014, 22(8): 890-897.
[25]	王金翠, 张英, 温吉利, 等. 华北平原气候时空演变特征[J]. 现代地质, 2015, 29(2): 299-306.
[26]	刘海燕, 刘茂涵, 张卫民, 等. 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. DOI
[27]	张小文, 何江涛, 黄冠星. 石家庄地区浅层地下水铁锰分布特征及影响因素分析[J]. 地学前缘, 2021, 28(4): 206-218. DOI
[28]	王仕琴, 郑文波, 孔晓乐. 华北农区浅层地下水硝酸盐分布特征及其空间差异性[J]. 中国生态农业学报, 2018, 26(10): 1476-1482.
[29]	张翠云, 张胜, 李政红, 等. 滹沱河上游区地表水和地下水同位素特征[J]. 干旱区资源与环境, 2008, 22(5): 160-164.
[30]	万长园, 王明玉, 王慧芳, 等. 华北平原典型剖面地下水三氮污染时空分布特征[J]. 地球与环境, 2014, 42(4): 472-479.
[31]	张兆吉, 费宇红, 陈宗宇, 等. 华北平原地下水可持续利用调查评价[M]. 北京: 地质出版社, 2009: 25-62.
[32]	林忠辉, 莫兴国. 历史时期黄淮海平原农作制度变迁与农业生产环境演变[J]. 中国生态农业学报, 2011, 19(5): 1072-1079.
[33]	敦宇, 许嘉文, 白雪山, 等. 地下水灌溉对华北平原农田土壤碳库转化影响[J]. 环境科学研究, 2021, 34(5): 1187-1195.
[34]	李晓欣, 马洪斌, 胡春胜, 等. 华北山前平原农田土壤硝态氮淋失与调控研究[J]. 中国生态农业学报, 2011, 19(5): 1109-1114.
[35]	张玉铭, 胡春胜, 毛任钊, 等. 华北山前平原农田土壤肥力演变与养分管理对策[J]. 中国生态农业学报, 2011, 19(5): 1143-1150.
[36]	梁慧雅, 王仕琴, 魏守才. 华北山前平原典型厚包气带硝态氮分布累积规律[J]. 土壤, 2017, 49(6): 1179-1186.
[37]	王茜, 沈彦俊, 裴宏伟, 等. 华北山前平原灌溉农田深层土壤水分动态特征及渗漏量估算[J]. 南水北调与水利科技, 2013, 11(1): 155-160.
[38]	裴宏伟, 沈彦俊, 刘昌明. 华北平原典型农田氮素与水分循环[J]. 应用生态学报, 2015, 26(1): 283-296.
[39]	袁志发, 周静芋. 多元统计分析[M]. 北京: 科学出版社, 2002.
[40]	刘学娜, 李海明, 李梦娣, 等. 天津平原区加油站地下水石油烃污染特征及其生物降解机理研究[J]. 地学前缘, 2022, 29(3): 227-238. DOI
[41]	RICHARDS L E, JOLLIFFE I T. Principal component analysis[J]. Journal of Marketing Research, 1988, 25(4): 410.
[42]	吕晓立, 郑跃军, 韩占涛, 等. 城镇化进程中珠江三角洲地区浅层地下水中砷分布特征及成因[J]. 地学前缘, 2022, 29(3): 88-98. DOI
[43]	吴娟娟, 卞建民, 万罕立, 等. 松嫩平原地下水氮污染健康风险评估[J]. 中国环境科学, 2019, 39(8): 3493-3500.
[44]	ZHANG Y T, WU J H, XU B. Human health risk assessment of groundwater nitrogen pollution in Jinghui canal irrigation area of the loess region, Northwest China[J]. Environmental Earth Sciences, 2018, 77(7): 1-12. DOI URL
[45]	MEANS B. Risk-assessment guidance for Superfund. Volume 1. Human health evaluation manual. Part A. Interim report (final)[R]. Washington: Office of Emergency and Remedial Response, US Environmental Protection Agency, 1989.
[46]	黄建洪, 张琴, 王晋昆, 等. 水环境污染健康风险评价中饮水量暴露参数的研究进展[J]. 卫生研究, 2021, 50(1): 146-153.
[47]	环境保护部. 中国人群暴露参数手册(成人卷)[M]. 北京: 中国环境出版社, 2013.
[48]	环境保护部. 中国人群暴露参数手册(儿童卷 0-5岁)[M]. 北京: 中国环境出版社, 2016.
[49]	环境保护部. 中国人群暴露参数手册(儿童卷 6-17岁)[M]. 北京: 中国环境出版社, 2016.
[50]	仲少鑫, 钱岩, 郭庶, 等. 空气污染物暴露人群活动模式研究进展[J]. 环境与健康杂志, 2019, 36(9): 836-842.
[51]	ZHAI Y Z, LEI Y, WU J, et al. Does the groundwater nitrate pollution in China pose a risk to human health? A critical review of published data[J]. Environmental Science and Pollution Research, 2017, 24(4): 3640-3653. DOI URL
[52]	GELBERG K H, CHURCH L, CASEY G, et al. Nitrate levels in drinking water in rural New York State[J]. Environmental Research, 1999, 80(1): 34-40. PMID
[53]	MAO H R, WANG G C, RAO Z, et al. Deciphering spatial pattern of groundwater chemistry and nitrogen pollution in Poyang Lake Basin (eastern China) using self-organizing map and multivariate statistics[J]. Journal of Cleaner Production, 2021, 329: 129697. DOI URL
[54]	LIU F, ZOU J W, LIU J R, et al. Factors controlling groundwater chemical evolution with the impact of reduced exploitation[J]. Catena, 2022, 214: 106261. DOI URL
[55]	GAO Z J, HAN C, YUAN S Y, et al. Assessment of the hydrochemistry, water quality, and human health risk of groundwater in the northwest of Nansi Lake Catchment, North China[J]. Environmental Geochemistry and Health, 2022, 44(3): 961-977. DOI
[56]	LIU J T, PENG Y M, LI C S, et al. Characterization of the hydrochemistry of water resources of the Weibei Plain, northern China, as well as an assessment of the risk of high groundwater nitrate levels to human health[J]. Environmental Pollution, 2021, 268: 115947. DOI URL
[57]	徐建国, 李生果, 朱恒华, 等. 南四湖流域平原区浅层地下水氮污染特征[J]. 工程勘察, 2010, 38(5): 40-44.
[58]	SOLDATOVA E, GUSEVA N, BYCHINSKY V. Modelling ofredox conditions in the shallow groundwater: a case study of agricultural areas in the Poyang Lake Basin, China[J]. Procedia Earth and Planetary Science, 2017, 17: 197-200. DOI URL
[59]	SU H, KANG W D, XU Y J, et al. Assessing groundwater quality and health risks of nitrogen pollution in the Shenfu mining area of Shaanxi Province, Northwest China[J]. Exposure and Health, 2018, 10(2): 77-97. DOI URL

华北平原典型山前冲洪积扇高硝态氮地下水分布特征及健康风险评价

Occurrences and health risks of high-nitrate groundwater in typical piedmont areas of the North China Plain

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 18

参考文献 59

相关文章 5

编辑推荐

Metrics

本文评价

[1]	黄柳琴, 李林鑫, 蒋宏忱. BIFs的形成及其铁氧化机制研究进展与展望[J]. 地学前缘, 2023, 30(2): 333-346.
[2]	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.
[3]	李志红, 王广才, 蔡五田, 刘菲, 黄丹丹. 某Cr(Ⅵ)污染场地修复的PRB反应材料及结构设计研究[J]. 地学前缘, 2021, 28(5): 186-196.
[4]	张小文, 何江涛, 黄冠星. 石家庄地区浅层地下水铁锰分布特征及影响因素分析[J]. 地学前缘, 2021, 28(4): 206-218.
[5]	刘淑琴，张尚军，牛茂斐，余力. 煤炭地下气化技术及其应用前景[J]. 地学前缘, 2016, 23(3): 97-102.