清水泉地下河多环芳烃来源及分配动态

王喆; 李江; 卢丽; 夏日元; 曹建文; 赵良杰; 栾松

doi:10.11932/karst2022y15

清水泉地下河多环芳烃来源及分配动态

doi: 10.11932/karst2022y15

王喆^{1, 2, 3,},
李江^1, ,,
卢丽^{2, 3},
夏日元^{2, 3},
曹建文^{2, 3},
赵良杰^{2, 3},
栾松^{2, 3}

1.
东华理工大学化学生物与材料科学学院, 江西南昌 330013
2.
中国地质科学院岩溶地质研究所,广西桂林 541004
3.
自然资源部、广西岩溶动力学重点实验室, 广西桂林 541004

基金项目: 广西重点研发计划项目（桂科AB22080070）；国家自然科学基金项目(41807218,41602277)；国家重点研发计划课题项目(2017YFC0406104)；中国地质调查局地质调查项目(DD20190342)

详细信息

作者简介:
王喆(1985—) ，男，硕士，助理研究员，主要从事岩溶水文地质环境地质研究。E-mail：wzhe@mail.cgs.gov.cn

通讯作者:
李江(1966—) ，男，教授，博士生导师，主要从事微生物冶金和微生物分子生物学研究。E-mail：li660001@163.com

中图分类号: X523
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出版历程
- 收稿日期: 2021-06-20
- 刊出日期: 2023-04-25

Dynamic research on source and distribution of PAHs in the Qingshuiquan underground river

WANG Zhe^{1, 2, 3
,},
LI Jiang^{1
, ,},
LU Li^{2, 3},
XIA Riyuan^{2, 3},
CAO Jianwen^{2, 3},
ZHAO Liangjie^{2, 3},
LUAN Song^{2, 3}

1.
School of Chemistry, Biology and Material Science, East China University of Technology, Nanchang, Jiangxi 330013, China
2.
Institute of Karst Geology, CAGS, Guilin, Guangxi 541004, China
3.
Key Laboratory of Karst Dynamics, MNR & GZAR, Guilin, Guangxi 541004, China

摘要

摘要: 城市化进程的不断加快，使得南宁市地下水多环芳烃（PAHs）污染日益严重，作为城市主要饮用水源地的清水泉地下河，对当地的经济和社会发展具有重要的支撑作用。文章选择南宁市清水泉地下河作为岩溶地下河的代表，以前人多年测试数据为基础，结合本次采样数据，分析水环境中PAHs的含量、分布特征和来源的多年变化情况，重点研究PAHs的分配规律。结果表明：地下水PAHs以2~3环为主，沉积物PAHs以4~6环为主，且由于污染源的增多，使得水环境中PAHs含量从上游到下游逐渐增大；不同区域的PAHs来源多年变化规律有差异，上游PAHs来源一直为生物质燃烧源，中游的PAHs来源由石油源转变为混合源，下游PAHs来源由以化石燃料燃烧源为主转变为以混合源为主；随着环数的增加，分配系数逐渐增加，且环数越大的PAHs更趋向被沉积物吸附；下游大部分采样点的PAHs在颗粒物上吸附能力较强，剩余采样点在分配过程中受溶解性有机质的影响。
- 多环芳烃 /
- 地下河 /
- 来源 /
- 分配 /
- 动态规律
Abstract: In recent years, the groundwater pollution of polycyclic aromatic hydrocarbons (PAHs) in Nanning City has been increasingly serious due to the acceleration of urbanization in this city and its dual water-bearing structure of underground and surface as well as the properties of PAHs. As a major source of drinking water for the city, the Qingshuiquan underground river plays an important role in the local economic and social development. Therefore, more research on PAHs pollution in Naning City is needed.Covering an area of about 55.3 km², the Qingshuiquan underground river is located in the northwest of Nanning. The strata distributed in the area are mainly upper Carboniferous (C3), Lower Cretaceous (K1) and Paleocene (E1), and the lithology is mostly thick bedded limestone. There are two underground river pipelines in the area. The groundwater mostly flows from east to west in the way of pipeline flow, and is discharged from the surface in the form of underground river outlet at S15 and flows into the Bachi river. At present, with an annual water supply capacity of 19 million square meters, the Qingshuiquan underground river provides drinking water for Yongning district of Nanning City, and is an important source of drinking water in Nanning City. In the upper reaches of the system, pollution is mainly from agricultural and domestic pollutants. In its middle and lower reaches, pollution is mainly generated from industrial enterprises, including cement plants, paper mills, quarries and gas stations.Based on the previous test data and the sampling data of this study, the research is mainly focused on the distribution rule of PAHs with the Qingshuiquan underground river as the research object. The statistics method, isomer ratio method, distribution coefficient method and others were adopted to analyze the content, distribution characteristics and source change of PAHs in water environment over the years. Results showed that, (1) The PAHs content with different ring numbers in groundwater were in the order of 4>3>5>2>6, mainly with low ring (2-3); the content of PAHs with different ring numbers in sediment were in the order of 4>5>3>6 >2, mainly with high ring (4-6). The PAHs content in groundwater experienced an increase after a decrease, but the content in sediment saw a gradual increase, which reflected different dynamic characteristics of PAHs content in groundwater and sediment due to the urbanization and industrialization in Nanning City. (2) The spatial distribution of PAHs content in water environment was listed as follows, upstream content<middle stream content<downstream content, which may be caused by the increase of industrial pollution sources as well as PAHs emissions from upstream to downstream. The variation trend of PAHs content in groundwater in different regions was different. The content of PAHs in groundwater increased gradually in the upstream, stabilized initially and then increased sharply in the middle, and decreased first and increased afterward in the downstream. The content of PAHs in sediments of different regions presented the same trend of a gradual increase, but the increase rate was different. (3) There are also differences between the change rules over the years. The PAHs sources at upstream reaches has been generated by biomass burning, and have changed from petroleum source to the mixed one at middle reaches. At downstream, the PAHs sources has changed from fossil fuel combustion to primarily mixed source. These changes are mainly attributed to different types of pollution sources and their emissions in different areas. (4) Kp values of different ring numbers were in the order of 6>5>4>3>2. Kp values gradually increased with rise of ring numbers, and PAHs with larger ring numbers tended to be adsorbed by sediments. The lgK_oc values of PAHs at S11-S15 sampling sites all exceeded the upper limit and were distributed in downstream, showing a strong adsorption capacity of PAHs on particulate matter. The lgK_oc values of the remaining sampling sites are below the upper limit, reflecting the influence of dissolved organic matter on the distribution of PAHs.
- polycyclic aromatic hydrocarbons /
- underground river /
- source /
- partition /
- dynamic law

HTML

图 1 清水泉地下河水文地质图

Figure 1. Hydrogeological map of the Qingshuiquan underground river

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图 2 地下水中∑₁₆PAHs含量分布多年变化情况

Figure 2. Variation of content distribution of ∑₁₆PAHs in groundwater

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图 3 沉积物中∑₁₆PAHs含量分布多年变化情况

Figure 3. Variation of content distribution of ∑₁₆PAHs in sediments

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图 4 采样点的lgK_oc与正辛醇—水分配系数lgK_ow的关系

Figure 4. Relationship between lgK_oc and lgK_ow of the sampling point

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表 1 同分异构体比值法判定PAHs来源的标准

Table 1. Standard for determining the sources of PAHs by isomer ratio method

PAHs比值	PAHs来源
FlA/(FlA+Pyr)	石油来源	石油类物质燃烧来源	草、木、煤燃烧来源
FlA/(FlA+Pyr)	<0.4	0.4~0.5	>0.5
BaA/(BaA+Chr)	石油来源	石油和燃烧混合来源	燃烧来源
BaA/(BaA+Chr)	<0.2	0.2~0.35	>0.35

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表 2 清水泉地下河∑₁₆PAHs含量

Table 2. Content of ∑₁₆PAHs in the Qingshuiquan underground river

PAHs	地下水/ng·L⁻¹			沉积物/ng·g⁻¹
PAHs	最小值	最大值	平均值	最小值	最大值	平均值
2环	32.57	58.78	47.50	27.01	50.26	34.96
3环	60.94	122.77	90.81	113.55	328.17	155.41
4环	87.76	225.14	122.40	132.16	428.58	254.28
5环	30.41	126.07	72.86	47.69	366.27	190.26
6环	9.43	48.77	23.66	28.29	173.66	88.54
∑₁₆PAHs	287.83	478.52	356.20	418.53	1232.23	721.51

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表 3 清水泉地下河∑₁₆PAHs含量多年变化情况

Table 3. Variation content of ∑₁₆PAHs in the Qingshuiquan underground river over the years

时间	2012年1月	2014年1月	2014年12月	2016年12月	2018年2月
地下水/ng·L⁻¹	220.98	170.50	191.71		356.20
沉积物/ng·g⁻¹		61.79		430.86	721.51

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表 4 清水泉地下河PAHs比值多年变化情况

Table 4. Variation of PAHs ratios in the Qingshuiquan underground river over the years

时间	PAHs比值	上游		中游		下游
时间	PAHs比值	范围	平均值	范围	平均值	范围	平均值
2012年1月	FLA/Pyr			1.97~2.13	2.05	0.86~1.47	1.07
2012年1月	BaA/BaA+Chr					0.36~0.62	0.52
2018年2月	FLA/FLA+Pyr	0.52~0.61	0.55	0.42~0.58	0.51	0.45~0.48	0.46
2018年2月	BaA/BaA+Chr	0.37~0.49	0.42	0.24~0.39	0.33	0.29~0.33	0.31

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表 5 不同环数PAHs的分配系数

Table 5. Partition coefficients of PAHs with different ring numbers

PAHs	Kp/L·g⁻¹
PAHs	最小值	最大值	平均值
2环	0.75	0.75	0.75
3环	1.54	1.92	1.78
4环	1.92	2.56	2.24
5环	2.25	3.53	2.40
6环	0.83	3.91	2.53
∑₁₆PAHs	0.75	3.91	2.37

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