22种药品与个人护理产品在河流中的污染特征研究

doi:10.16258/j.cnki.1674-5906.2022.06.016

生态环境学报 ›› 2022, Vol. 31 ›› Issue (6): 1200-1207.DOI: 10.16258/j.cnki.1674-5906.2022.06.016

22种药品与个人护理产品在河流中的污染特征研究

潘丹琳(), 王飞飞^*(), 曹文志, 陈一悦

厦门大学滨海湿地生态系统教育部重点实验室/厦门大学环境与生态学院,福建厦门 361102

收稿日期:2021-08-01 出版日期:2022-06-18 发布日期:2022-07-29
通讯作者: *王飞飞,E-mail: feifeiw@xmu.edu.cn
作者简介:潘丹琳（1996年生）,女,硕士研究生,研究方向为河流污染特征研究。E-mail: 452350387@qq.com
基金资助:
广西科技重大专项(桂科AA17202032);福建省环保科技计划项目(2021R023)

The Study on Characteristics of 22 Pharmaceuticals and Personal Care Products in Rivers

PAN Danlin(), WANG Feifei^*(), CAO Wenzhi, CHEN Yiyue

Key Laboratory of the Ministry of Education for Coastal and Wetland Ecosystems/College of the Environment and Ecology, Xiamen University, Xiamen 361102, P. R. China

Received:2021-08-01 Online:2022-06-18 Published:2022-07-29

摘要/Abstract

摘要：

新污染物药物和个人护理产品（PPCPs）对环境具有潜在影响,近年来引起了广泛的关注。由于环境中各类PPCPs的含量受到多种因素的影响,在不同流域与地区均存在一定差异。收集、整理了国内外60个典型流域22种目标PPCPs的检出频率和质量浓度数据,并筛选出PPCPs污染来源的指示物。结果表明,60个流域中22种目标PPCPs的检出频率超过或接近50%的包括CBZ、SMX、CAF、ERY、IPF和NPX,其中,CBZ在国内外的检出率均为最高。CAF、BPA、KTP等13种PPCPs的最大检出质量浓度超过了μg∙L^-1数量级。国内的目标PPCPs检出类别少于国外,且检出质量浓度水平总体上低于国外,但OFX（ND—7632 ng∙L^-1）、SMR（ND—18.9 ng∙L^-1）和SA（26.3—2014.7 ng∙L^-1）的检出质量浓度高于国外平均水平,NFX、TMP的平均质量浓度与国外相当。结合各流域主要污染源特征及检出质量浓度,利用不稳定与稳定的PPCPs种类质量浓度的比值分析各流域污染特征。筛选国内外具有较高检出频率和质量浓度,并且具有相对稳定性的CBZ,作为稳定PPCPs的指示物,进而选择CAF/CBZ、SMX/CBZ、BPA/CBZ分别作为生活源（K_d）、农业源（K_a）和工业源（K_i）的指示指标,并推荐CAF/CBZ=10作为一个判断流域生活污水处理效率的潜在阈值。从30个生活源为主要污染来源流域的K_d值可以发现,国内流域的生活源源强比国外大,说明生活污水处理率整体上低于国外处理水平。K_d值可以作为评估流域污水处理效率的有效指标,同时初步提出了K值作为不同污染源强和污染特征的指示指标,可以为评估流域污染来源和污染状况提供参考和新的思路。

关键词: PPCPs, 检出率, 检出质量浓度, 污染源, 不稳定与稳定PPCPs的比值, 评估指标

Abstract:

Emerging pollutants represented by pharmaceuticals and personal care products (PPCPs) have attracted widespread attention in recent years due to their potential impacts on the environment and human health. As the concentrations of PPCPs in the environment are affected by many factors, they varied in different river basins and regions. This study collected and sorted out the detection frequency and mass concentrations of 22 target PPCPs from 60 typical watersheds in China and other countries, and screened out some PPCPs as indicators of different pollution sources. The results showed that the detection frequency of some PPCPs in 60 basins was over or close to 50%, including CBZ, SMX, CAF, ERY, IPF and NPX, among which, CBZ had the highest detection rates in China and abroad. The maximum concentrations of 13 kinds of PPCPs, including CAF, BPA and KTP, exceeded the magnitude of μg·L^-1. The species of target PPCPs detected in China was less than those in foreign countries, and the concentration level of target PPCPs detected in China was generally lower than that in foreign countries. However, OFX (ND-7632 ng∙L^-1), SMR (ND-18.9 ng∙L^-1) and SA (26.3-2014.7 ng∙L^-1) were higher than foreign averagely, while the average concentrations of NFX and TMP were similar to those of foreign countries. Combined with the characteristics of main pollution sources and detected mass concentrations from each watershed, the pollution characteristics of each watershed were analyzed by using the ratios of unstable and stable PPCPs mass concentrations. CBZ was screened as indicators of stable PPCPs due to its high detection frequency, high mass concentrations, and relative stability throughout all countries. Thus, the ratios of CAF/CBZ, SMX/CBZ and BPA/CBZ were selected as the indicators of domestic sewage source (K_d), agricultural (K_a) and industrial sources (K_i), respectively. The ratio of CAF/CBZ=10 was recommended as a potential threshold to judge the performance of domestic sewage treatment in watersheds. Based on the K_d value of thirty domestic sewage source watersheds, the results showed that the domestic sewage source was larger than that from watershed in foreign countries, indicating that the domestic sewage treatment rates were generally lower than those from watershed in foreign countries. K_d value can be used as an effective tool to evaluate the performance of sewage treatment in a watershed. Meanwhile, K values is proposed as an indicator for different pollution intensity and characteristics in watersheds, and this can provide reference and new thoughts for assessing the pollution sources and pollution status in a river watershed.

Key words: PPCPs, detection frequency, detection concentrations, pollution characteristics, ratio of unstable to stable PPCPs, evaluation indicators

中图分类号:

潘丹琳, 王飞飞, 曹文志, 陈一悦. 22种药品与个人护理产品在河流中的污染特征研究[J]. 生态环境学报, 2022, 31(6): 1200-1207.

PAN Danlin, WANG Feifei, CAO Wenzhi, CHEN Yiyue. The Study on Characteristics of 22 Pharmaceuticals and Personal Care Products in Rivers[J]. Ecology and Environment, 2022, 31(6): 1200-1207.

图/表 7

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序号 No.	名称 Name	英文 (缩写) English name (abbreviation)	类别 Classification
1	布洛芬	Ibuprofen (IPF)	镇痛消炎药
2	酮洛芬	Ketoprofen (KTP)	镇痛消炎药
3	水杨酸	Salicylic acid (SA)	消炎药
4	茶碱	Theophylline (TPL)	拮抗剂
5	卡马西平	Carbamazepine (CBZ)	抗癫痫药
6	普利米酮	Primidone (PMD)	抗癫痫药
7	萘普生	Naproxen (NPX)	激素
8	红霉素	Erythromycin (ERY)	抗生素类
9	环丙沙星	Ciprofloxacin (CFX)	抗生素类
10	诺氟沙星	Norfloxacin (NFX)	抗生素类
11	氧氟沙星	Ofloxacin (OFX)	抗生素类
12	磺胺甲恶唑	Sulfamethoxazole (SMX)	抗生素类
13	磺胺甲基嘧啶	Sulfamerazine (SMR)	抗生素类
14	氯霉素	Chloramphenicol (CPN)	抗生素类
15	甲氧苄啶	Trimethoprim (TMP)	抗菌类药物
16	硝酸咪康唑	Miconazole Nitrate (MCN)	抗菌类药物
17	氟康唑	Fluconazole (FCZ)	抗菌类药物
18	三氯卡班	Triclocarban (TCC)	抗菌药物/消毒剂
19	吉非罗齐	Gemfibrozil (GFZ)	血脂调节剂
20	羟苯甲酯	Methylparaben (MPB)	杀菌防腐剂
21	咖啡因	Caffeine (CAF)	精神兴奋剂
22	双酚A	Bisphenol A (BPA)	增塑剂

序号 No.	名称 Name	英文 (缩写) English name (abbreviation)	类别 Classification
1	布洛芬	Ibuprofen (IPF)	镇痛消炎药
2	酮洛芬	Ketoprofen (KTP)	镇痛消炎药
3	水杨酸	Salicylic acid (SA)	消炎药
4	茶碱	Theophylline (TPL)	拮抗剂
5	卡马西平	Carbamazepine (CBZ)	抗癫痫药
6	普利米酮	Primidone (PMD)	抗癫痫药
7	萘普生	Naproxen (NPX)	激素
8	红霉素	Erythromycin (ERY)	抗生素类
9	环丙沙星	Ciprofloxacin (CFX)	抗生素类
10	诺氟沙星	Norfloxacin (NFX)	抗生素类
11	氧氟沙星	Ofloxacin (OFX)	抗生素类
12	磺胺甲恶唑	Sulfamethoxazole (SMX)	抗生素类
13	磺胺甲基嘧啶	Sulfamerazine (SMR)	抗生素类
14	氯霉素	Chloramphenicol (CPN)	抗生素类
15	甲氧苄啶	Trimethoprim (TMP)	抗菌类药物
16	硝酸咪康唑	Miconazole Nitrate (MCN)	抗菌类药物
17	氟康唑	Fluconazole (FCZ)	抗菌类药物
18	三氯卡班	Triclocarban (TCC)	抗菌药物/消毒剂
19	吉非罗齐	Gemfibrozil (GFZ)	血脂调节剂
20	羟苯甲酯	Methylparaben (MPB)	杀菌防腐剂
21	咖啡因	Caffeine (CAF)	精神兴奋剂
22	双酚A	Bisphenol A (BPA)	增塑剂

序号 No.	流域 River basin	主要污染源 The main pollution sources	参考文献 References
1	九龙江	畜禽养殖、农业种植	Lü et al., 2014
2	珠江广州段	生活污水	Yang et al., 2011
3	长江中下游地区	生活污水、工业废水	Kasprzyk-Hordern et al., 2008; Yang et al., 2011; Zhou et al., 2011; Daneshvar et al., 2012; Lü et al., 2014; Wu et al., 2014; Nakada et al., 2017
4	鄱阳湖	农业种植、生活污水
5	洞庭湖	畜禽养殖、生活污水
6	太湖	生活污水
7	巢湖	工业废水
8	基隆河	生活污水	Pai et al., 2020
9	骆马湖	水产养殖	陈宇等, 2020
10	汉江	工业废水	高月等, 2018
11	白洋淀	生活污水	Li et al., 2010
12	北运河天津段	生活污水	胡伟, 2011
13	海河	生活污水、农业污水	Wang et al., 2010
14	蓟运河	畜禽养殖	Zhang et al., 2014
15	南运河天津段	生活污水、农业污水	胡伟, 2011
16	清河	农业污水	卫毅梅, 2013
17	黄浦江	工业废水、生活污水	Wu et al., 2013
18	黄河三角洲	水产养殖	Zhao et al., 2016
19	淮河	工业废水	Zhang et al., 2013
20	三亚主要河流	生活污水、畜禽养殖	任丙南等, 2021
21	潮白河	生活污水、工业废水	刘娴静等, 2021
22	北部湾	生活污水	Zheng et al., 2012
23	黄海盐城段	生活污水、畜禽养殖	Du et al., 2017
24	钦州湾	生活污水	Cui et al., 2019
25	辽东湾	生活污水、畜禽养殖	Jia et al., 2011
26	香港新界主要河流	生活污水、农业污水	Deng et al., 2016
27	Thames River, England	生活污水	Papageorgiou et al., 2016
28	Riverside County, California	生活污水	Yu et al., 2013
29	Illinois, USA	生活污水	Li et al., 2013
30	Karnataka, India	生活污水	Balakrishna et al., 2017
31	the northwest of Spain	生活污水	Reyes-Contreras et al., 2012
32	Texas, USA	生活污水	Oppenheimer et al., 2011
33	Pagasetic Gulf, Greece	生活污水	Papageorgiou et al., 2016
34	RhôneeAlpes, France	生活污水	Vulliet et al., 2011
35	French groundwater	工业废水	Lopez et al., 2015
36	Ottawa, Ontario, Canada	农业种植	Gottschall et al., 2012
37	Besòs River, Spain	生活污水、农业污水	Lopez-Serna et al., 2013
38	Llobregat delta, Spain	生活污水	Cabeza et al., 2012
39	Cau River, Vietnam	生活污水	Ngo et al., 2021
40	Mankyung River, South Korea	农业种植	Kim et al., 2009
41	Somes River, Romania	生活污水	Moldovan, 2006
42	Apies River, South Africa	生活污水	Mhuka et al., 2020
43	Indus River, Pakistan	农业种植	Khan et al., 2013
44	Taff River, South Wales, UK	生活污水	Kasprzyk-Hordern et al., 2008
45	Ely River, South Wales, UK	生活污水	Kasprzyk-Hordern et al., 2008
46	Lis River, Portugal	生活污水、畜禽养殖	Paiga et al., 2016
47	Ganges River, India	生活污水	Singh et al., 2021
48	Michigan Lake, USA	生活污水、工业废水	Blair et al., 2013
49	Buyukcekmece Lake, Turkey	生活污水	Aydin et al., 2013
50	Kraków, Poland	生活污水	Rusiniak et al., 2021
51	drinking water in the USA	生活污染	Benotti et al., 2009
52	Albufera Natural Park, Spain	农业种植	Sadutto et al., 2021
53	Bacanga River, Brazil	生活污水	Silva Chaves et al., 2020
54	Red Sea, the Saudi Arabia	工业废水、生活污水	Ali et al., 2017
55	Seine River, France	生活污水	Tamtam et al., 2008
56	Ebro River, Spain	农业种植	da Silva et al., 2011
57	Choptank River Watershed, Maryland, USA	农业种植	Arikan et al., 2008
58	the Po Valley, Italy	生活污水	Al Aukidy et al., 2012
59	Trentino-Alto Adige region, Italy	生活污水	Mandaric et al., 2017
60	Krajkowo-Poznan, Poland	生活污水	Kruc et al., 2019

序号 No.	流域 River basin	主要污染源 The main pollution sources	参考文献 References
1	九龙江	畜禽养殖、农业种植	Lü et al., 2014
2	珠江广州段	生活污水	Yang et al., 2011
3	长江中下游地区	生活污水、工业废水	Kasprzyk-Hordern et al., 2008; Yang et al., 2011; Zhou et al., 2011; Daneshvar et al., 2012; Lü et al., 2014; Wu et al., 2014; Nakada et al., 2017
4	鄱阳湖	农业种植、生活污水
5	洞庭湖	畜禽养殖、生活污水
6	太湖	生活污水
7	巢湖	工业废水
8	基隆河	生活污水	Pai et al., 2020
9	骆马湖	水产养殖	陈宇等, 2020
10	汉江	工业废水	高月等, 2018
11	白洋淀	生活污水	Li et al., 2010
12	北运河天津段	生活污水	胡伟, 2011
13	海河	生活污水、农业污水	Wang et al., 2010
14	蓟运河	畜禽养殖	Zhang et al., 2014
15	南运河天津段	生活污水、农业污水	胡伟, 2011
16	清河	农业污水	卫毅梅, 2013
17	黄浦江	工业废水、生活污水	Wu et al., 2013
18	黄河三角洲	水产养殖	Zhao et al., 2016
19	淮河	工业废水	Zhang et al., 2013
20	三亚主要河流	生活污水、畜禽养殖	任丙南等, 2021
21	潮白河	生活污水、工业废水	刘娴静等, 2021
22	北部湾	生活污水	Zheng et al., 2012
23	黄海盐城段	生活污水、畜禽养殖	Du et al., 2017
24	钦州湾	生活污水	Cui et al., 2019
25	辽东湾	生活污水、畜禽养殖	Jia et al., 2011
26	香港新界主要河流	生活污水、农业污水	Deng et al., 2016
27	Thames River, England	生活污水	Papageorgiou et al., 2016
28	Riverside County, California	生活污水	Yu et al., 2013
29	Illinois, USA	生活污水	Li et al., 2013
30	Karnataka, India	生活污水	Balakrishna et al., 2017
31	the northwest of Spain	生活污水	Reyes-Contreras et al., 2012
32	Texas, USA	生活污水	Oppenheimer et al., 2011
33	Pagasetic Gulf, Greece	生活污水	Papageorgiou et al., 2016
34	RhôneeAlpes, France	生活污水	Vulliet et al., 2011
35	French groundwater	工业废水	Lopez et al., 2015
36	Ottawa, Ontario, Canada	农业种植	Gottschall et al., 2012
37	Besòs River, Spain	生活污水、农业污水	Lopez-Serna et al., 2013
38	Llobregat delta, Spain	生活污水	Cabeza et al., 2012
39	Cau River, Vietnam	生活污水	Ngo et al., 2021
40	Mankyung River, South Korea	农业种植	Kim et al., 2009
41	Somes River, Romania	生活污水	Moldovan, 2006
42	Apies River, South Africa	生活污水	Mhuka et al., 2020
43	Indus River, Pakistan	农业种植	Khan et al., 2013
44	Taff River, South Wales, UK	生活污水	Kasprzyk-Hordern et al., 2008
45	Ely River, South Wales, UK	生活污水	Kasprzyk-Hordern et al., 2008
46	Lis River, Portugal	生活污水、畜禽养殖	Paiga et al., 2016
47	Ganges River, India	生活污水	Singh et al., 2021
48	Michigan Lake, USA	生活污水、工业废水	Blair et al., 2013
49	Buyukcekmece Lake, Turkey	生活污水	Aydin et al., 2013
50	Kraków, Poland	生活污水	Rusiniak et al., 2021
51	drinking water in the USA	生活污染	Benotti et al., 2009
52	Albufera Natural Park, Spain	农业种植	Sadutto et al., 2021
53	Bacanga River, Brazil	生活污水	Silva Chaves et al., 2020
54	Red Sea, the Saudi Arabia	工业废水、生活污水	Ali et al., 2017
55	Seine River, France	生活污水	Tamtam et al., 2008
56	Ebro River, Spain	农业种植	da Silva et al., 2011
57	Choptank River Watershed, Maryland, USA	农业种植	Arikan et al., 2008
58	the Po Valley, Italy	生活污水	Al Aukidy et al., 2012
59	Trentino-Alto Adige region, Italy	生活污水	Mandaric et al., 2017
60	Krajkowo-Poznan, Poland	生活污水	Kruc et al., 2019

生活源比值 Ratio of domestic source	流域 River basin	比值范围 Ranges of ratio	参考文献 References
CAF/CBZ	Thames River	0.1-100	Nakada et al., 2017
	九龙江	1-141	Lü et al.,2014
	钦州湾	10-50	Cui et al., 2019
	通惠河	1-20	Ma et al., 2016
	洞庭湖	11-103.4	Ma et al., 2016
	清河	10-80	Ma et al., 2017
	北运河	0.7-70	Ma et al., 2017

22种药品与个人护理产品在河流中的污染特征研究

The Study on Characteristics of 22 Pharmaceuticals and Personal Care Products in Rivers

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污染源 Pollution sources	比值 Ratio	含义 Implication	国内 China		国外 Other countries
污染源 Pollution sources	比值 Ratio	含义 Implication	范围 Ranges	平均值±标准差 Average±SD	范围 Ranges	平均值±标准差 Average±SD
生活源 (K_d) Domestic source	CAF/CBZ 或IPF/CBZ	比值小表示源强小、直排现象越少、污水处理效率越高;比值大表示源强大、污水处理效率低、污水存在直排等	0.1-393	70.82±94.11	0.25-246.6	41.64±60.30
农业源 (K_a) Agricultural source	SMX/CBZ	比值小表示农业源污染较低;比值大表示农业源污染程度严重,可能存在非点源污染	0.19-584.44	43.92±95.30	0.05-122	5.95±14.67
工业源 (K_i) Industrial source	BPA/CBZ 或ERY/CBZ	比值小表示工业污染源强小,处理率高; 反之,表示源强大、处理率低	0.37-83.88	22.80±25.97	1.71-144.4	33.78±46.19