华南滨海小流域地下水中PPCPs的分布、来源及影响因素——以珠海市唐家湾镇为例

doi:10.16258/j.cnki.1674-5906.2024.02.009

生态环境学报 ›› 2024, Vol. 33 ›› Issue (2): 249-260.DOI: 10.16258/j.cnki.1674-5906.2024.02.009

• 研究论文【环境科学】 • 上一篇下一篇

华南滨海小流域地下水中PPCPs的分布、来源及影响因素——以珠海市唐家湾镇为例

梁贝竹¹(), 陈建耀¹^,^*, 杨再智¹, 张鹏程¹, 任坤¹, 梁作兵¹, 杨晨晨¹, 吴洁珊²

1.中山大学地理科学与规划学院，广东广州 510006
2.拱北海关技术中心，广东珠海 519020

收稿日期:2023-08-31 出版日期:2024-02-18 发布日期:2024-04-03
通讯作者: *陈建耀。
作者简介:梁贝竹（2001年生），女，硕士研究生，研究方向为流域水环境。E-mail: liangbzh3@mail2.sysu.edu.cn
基金资助:
国家重点研发项目(2023YFC3709002);国家自然科学基金项目(41977171)

Spatial Pattern and Sources of PPCPs in Groundwater and Relevant Influencing Factors in a Coastal Watershed in South China: A Case Study in Tangjiawan Town of Zhuhai, Guangdong Province

LIANG Beizhu¹(), CHEN Jianyao¹^,^*, YANG Zaizhi¹, ZHANG Pengcheng¹, REN Kun¹, LIANG Zuobing¹, YANG Chenchen¹, WU Jieshan²

1. School of Geography and Planning, Sun Yat-sen University, Guangzhou 510006, P. R. China
2. Gongbei Customs District P. R. China Technical Center, Zhuhai 519020, P. R. China

Received:2023-08-31 Online:2024-02-18 Published:2024-04-03

摘要/Abstract

摘要：

药物和个人护理用品（Pharmaceutical and Personal Care Products，PPCPs）是在环境中长期存在并对人类乃至整个生态系统的健康造成威胁的两类化学消费品。珠江三角洲流域PPCPs的检出水平总体较高，沿海地区地下水中的PPCPs污染有待进一步探究。于2021年9月在珠海市唐家湾镇采集了16个地下水样本，使用LC-MS/MS分析技术对21种PPCPs进行检测，使用数理统计方法和相关性分析对研究区地下水中PPCPs浓度特征和污染来源进行解析，并结合地下水化学特征及统计分析对其影响因素进行探究，旨在为滨海地区地下水的PPCPs特征分析提供案例依据。研究发现，1）研究区地下水呈弱酸至弱碱性，水化学类型多属于HCO₃-Ca型，沿地下水流方向受人为污染的影响越来越显著。2）研究区地下水中检测到6种PPCPs，平均质量浓度和检出率分别为：磺胺甲恶唑（5.51 ng∙L⁻¹，81%）、磺胺甲基嘧啶（1.18 ng∙L⁻¹，100%）、磺胺二甲基嘧啶（0.168 ng∙L⁻¹，25%）、卡马西平（35.7 ng∙L⁻¹，94%）、咖啡因（110 ng∙L⁻¹，100%）、西马特罗（0.100 ng∙L⁻¹，6%）；磺胺类化合物和卡马西平从补给区到排泄区整体污染情况加重，存在一定累积效应，而咖啡因无明显的空间分布规律；可以将卡马西平视作研究区内PPCPs总体污染的潜在标志物。3）研究区地下水PPCPs属于农业和城镇活动的混合来源；磺胺二甲基嘧啶与水温呈显著正相关（P<0.05），与代谢菌群的繁殖和吸附过程有关；磺胺甲基嘧啶和咖啡因均与溶解氧呈显著负相关（P <0.05），与化粪池污水输入有关。综上所述，研究区地下水受到人类活动污染的程度较高，农业和城镇活动将大量PPCPs引入到地下水当中。

关键词: 地下水, PPCPs, 来源, 空间分布, 滨海小流域, 华南地区

Abstract:

Pharmaceutical and Personal Care Products (PPCPs) pose a threat to the health of human beings and whole ecosystem due to their long-term existence in the environment. The concentrations of PPCPs in the Pearl River Delta Basin are generally high, and few studies have been carried out for the PPCPs in groundwater in coastal areas. Sixteen groundwater samples in Tangjiawan Town, Zhuhai City were collected in September 2021, with PPCPs components analyzed by LC-MS/MS. Spatial pattern and sources of PPCPs in groundwater were identified by using statistical approaches, and the influencing factors were recognized by hydrochemical characteristics analysis. The results showed that: 1) The groundwater in the study area was weakly acidic or alkaline, and could be mostly classified as HCO₃-Ca type, with an increasing influence of anthropogenic pollutants following the groundwater flow from the recharge area to the discharge area. 2) Six compounds of PPCPs were detected in groundwater, and the average concentration and detection rate were given as follows: 5.51 ng∙L⁻¹, 81% for sulfamethoxazole, 1.18 ng∙L⁻¹, 100% for sulfamerazine, 0.168 ng∙L⁻¹, 25% for sulfamethazine, 35.7 ng∙L⁻¹, 94% for carbamazepine, 110 ng∙L⁻¹, 100% for caffeine, and 0.100 ng∙L⁻¹, 6% for cimatrol, respectively. The concentrations of sulfonamides and carbamazepine increased generally from the recharge area to the discharge area with a cumulative trend, and carbamazepine could be considered as a potential marker of PPCPs contamination in the study area, while no spatial pattern was found for caffeine. 3) Agricultural pesticides and human waste were mixed and contributed to PPCPs in groundwater. There was a significant positive correlation between sulfamethazine and temperature (P<0.05), attributing to the propagation of metabolic bacteria and adsorption process. Both sulfamerazine and caffeine were significantly negatively correlated with dissolved oxygen (P<0.05), which was closely related to the leakage of septic tank to the aquifer. The results can be used for the groundwater protection in the study area, and provide scientific base for managing groundwater resources.

Key words: groundwater, PPCPs, sources, spatial pattern, coastal watershed, south China

中图分类号:

梁贝竹, 陈建耀, 杨再智, 张鹏程, 任坤, 梁作兵, 杨晨晨, 吴洁珊. 华南滨海小流域地下水中PPCPs的分布、来源及影响因素——以珠海市唐家湾镇为例[J]. 生态环境学报, 2024, 33(2): 249-260.

LIANG Beizhu, CHEN Jianyao, YANG Zaizhi, ZHANG Pengcheng, REN Kun, LIANG Zuobing, YANG Chenchen, WU Jieshan. Spatial Pattern and Sources of PPCPs in Groundwater and Relevant Influencing Factors in a Coastal Watershed in South China: A Case Study in Tangjiawan Town of Zhuhai, Guangdong Province[J]. Ecology and Environment, 2024, 33(2): 249-260.

图/表 15

图1 水体中PPCPs的来源（Li et al.，2021）

Figure 1 Sources of PPCPs in water bodies (Li et al., 2021)

图2 珠海市唐家湾镇采样井分布（土地利用背景来自 (Li et al., 2023)）基于自然资源部标准地图服务网站GS (2016) 1600号标准地图制作，底图边界无修改

Figure 2 Distribution of sampling wells in Tangjiawan Town, Zhuhai City (Land use background from (Li et al., 2023) )

表1 珠海市唐家湾镇采样井概况

Table 1 Characteristics of sampling wells in Tangjiawan Town, Zhuhai City

采样井	纬度	经度
TJ01	22.3644°N	113.5877°E
TJ02	22.3638°N	113.5878°E
TJ03	22.3636°N	113.5881°E
TJ04	22.3636°N	113.5889°E
TJ05	22.3636°N	113.5883°E
TJ06	22.3636°N	113.5898°E
TJ07	22.3631°N	113.5897°E
TJ08	22.3626°N	113.5889°E
TJ09	22.3622°N	113.5883°E
TJ10	22.3625°N	113.5878°E
TJ11	22.3628°N	113.5881°E
TJ12	22.3622°N	113.5897°E
TJ13	22.3625°N	113.5906°E
TJ14	22.3628°N	113.5903°E
TJ15	22.3631°N	113.5922°E
TJSQS	22.3608°N	113.5818°E

图3 珠海市唐家湾镇地下水位等值线图地下水位等值线为海平面以上，单位：m

Figure 3 The contour map of groundwater level in Tangjiawan town, Zhuhai City

表2 珠海市唐家湾镇地下水基本理化参数统计特征值

Table 2 Statistical characteristic of physicochemical parameters of groundwater in Tangjiawan Town, Zhuhai City

统计指标	电导率/ (μS∙cm⁻¹)	溶解性总固体/ (mg∙L⁻¹)	盐度/ (mg∙L⁻¹)	溶解氧/ (mg∙L⁻¹)	pH
最小值	54.1	40.1	23.8	0.850	5.79
最大值	600	462	272	7.04	8.43
平均值	386	291	174	3.29	7.01
标准差	154	126	70.6	1.96	0.710
变异系数/%	40.0	43.4	40.5	59.5	10.1

图4 珠海市唐家湾镇地下水基本理化参数空间变化趋势 n=16。下同

Figure 4 Spatial variation trend of physicochemical parameters of groundwater in Tangjiawan Town, Zhuhai City

表3 珠海市唐家湾镇地下水离子质量浓度统计特征值

Table 3 Statistical characteristic of ionic concentration in groundwater in Tangjiawan Town, Zhuhai City

统计指标	ρ(K⁺)	ρ(Na⁺)	ρ(Ca²⁺)	ρ(Mg²⁺)	ρ(Cl⁻)	ρ(SO₄²⁻)	ρ(HCO₃⁻)
最小值/ (mg∙L⁻¹)	3.93	7.27	1.26	0.520	5.65	1.06	30.5
最大值/ (mg∙L⁻¹)	64.8	51.3	96.4	7.27	87.7	69.7	317
平均值/ (mg∙L⁻¹)	36.4	31.6	55.9	4.69	42.1	41.2	157
标准差/ (mg∙L⁻¹)	17.3	13.4	27.3	1.96	20.7	19.7	84.3
变异系数/%	47.6	42.6	48.9	41.8	49.2	47.7	53.8

图5 珠海市唐家湾镇地下水Cl?质量浓度与NO3?/Cl?摩尔比值的关系

Figure 5 Relationship between Cl? mass concentration and NO3?/Cl? molar ratio of groundwater in Tangjiawan Town, Zhuhai City

图6 珠海市唐家湾镇地下水Piper图

Figure 6 Piper map of groundwater in Tangjiawan Town, Zhuhai City

表4 珠海市唐家湾镇地下水PPCPs检出情况

Table 4 Detection condition of PPCPs in groundwater in Tangjiawan Town, Zhuhai City

PPCPs种类	质量浓度范围/ (ng∙L⁻¹)	中间值/ (ng∙L⁻¹)	均值/ (ng∙L⁻¹)	检出率/ %
Sulfadimethoxine 磺胺间二甲氧嘧啶	ND	0	0	0
Sulfamethoxazole 磺胺甲恶唑	ND‒58.6	29.3	5.51	81.0
Sulfamonomethoxine 磺胺间甲氧嘧啶	ND	0	0	0
Sulfamerazine 磺胺甲基嘧啶	0.919‒1.60	1.26	1.18	100
Sulfamethazine 磺胺二甲基嘧啶	ND‒0.883	0.442	0.168	25.0
Sulfachinoxalin 磺胺喹恶啉	ND	0	0	0
Tracycline 四环素	ND	0	0	0
Oxytetracycline 土霉素	ND	0	0	0
Chlorotetracycline 金霉素	ND	0	0	0
Doxycycline 强力霉素	ND	0	0	0
Enrofloxacin 恩诺沙星	ND	0	0	0
Ciprofloxacin 环丙沙星	ND	0	0	0
Clenbuterol 克伦特罗	ND	0	0	0
Salbutamol 沙丁氨醇	ND	0	0	0
Cimaterol 西马特罗	ND‒1.54	0.770	0.100	6.25
Ractopamine 莱克多巴胺	ND	0	0	0
Carbamazepine 卡马西平	ND‒334	167	35.7	93.8
Caffeine 咖啡因	6.49‒214	110	110	100
Atrazine 阿特拉津	ND	0	0	0
Chloramphenicol 氯霉素	ND	0	0	0
Florfenicol 氟苯尼考	ND	0	0	0

表5 珠海市唐家湾镇地下水PPCPs总量与单个PPCPs的关系

Table 5 The relationship between total PPCPs and individual PPCPs of groundwater in Tangjiawan Town, Zhuhai City

PPCPs	Pearson相关性	P值 (双侧显著性)
磺胺甲恶唑	−0.140	0.518
磺胺甲基嘧啶	0.452	0.083
磺胺二甲基嘧啶	0.394	0.878
西马特罗	−0.165	‒
卡马西平	0.839	0.000^*
咖啡因	0.540	0.061

图7 珠海市唐家湾镇地下水主要PPCPs空间分布特征

Figure 7 Spatial patterns of PPCPs in groundwater in Tangjiawan Town, Zhuhai City

图8 珠海市唐家湾镇地下水PPCPs聚类热图 SMX磺胺甲恶唑，SMR磺胺甲基嘧啶，SMZ磺胺二甲基嘧啶，CBZ卡马西平，CAF咖啡因

Figure 8 Clustering heat map of PPCPs in groundwater in Tangjiawan Town, Zhuhai City

图9 珠海市唐家湾镇土地利用（Li et al.，2023）与潜在污染源分布图

Figure 9 Land use (Li et al., 2023) and potential pollution sources map in Tangjiawan Town, Zhuhai City

图10 珠海市唐家湾镇地下水PPCPs与基本理化参数的相关性热图 SMX磺胺甲恶唑，SMR磺胺甲基嘧啶，SMZ磺胺二甲基嘧啶，CL西马特罗，CBZ卡马西平，CAF咖啡因；***表示P<0.001，**表示P<0.01，*表示P<0.05；n=16

Figure 10 Correlation heat map of PPCPs and physicochemical parameters of groundwater in Tangjiawan Town, Zhuhai City

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华南滨海小流域地下水中PPCPs的分布、来源及影响因素——以珠海市唐家湾镇为例

Spatial Pattern and Sources of PPCPs in Groundwater and Relevant Influencing Factors in a Coastal Watershed in South China: A Case Study in Tangjiawan Town of Zhuhai, Guangdong Province

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