Please wait a minute...
 首页  期刊列表 期刊订阅 开放获取 关于我们
English
最新录用  |  在线预览  |  当期目录  |  过刊浏览  |  学科浏览  |  专题文章  |  热点文章  |  下载排行
Frontiers of Environmental Science & Engineering    2020, Vol. 14 Issue (1) : 8-     https://doi.org/10.1007/s11783-019-1187-3
RESEARCH ARTICLE
Determination of 27 pharmaceuticals and personal care products (PPCPs) in water: The benefit of isotope dilution
Xueqi Fan1, Jie Gao1, Wenchao Li2, Jun Huang1(), Gang Yu1
1. State Key Joint Laboratory of Environment Simulation and Pollution Control (SKJLESPC), Beijing Key Laboratory for Emerging Organic Contaminants Control (BKLEOC), School of Environment, Tsinghua University, Beijing 100084, China
2. CSD IDEA (Beijing) Environment Test & Analysis Co., Ltd., Beijing 100192, China
全文: PDF(787 KB)   HTML
导出: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

• Isotope dilution method was developed for the determination of 27 PPCPs in water.

• The established method was successfully applied to different types of water samples.

• The correction effect of corresponding 27 ILSs over 70 d was investigated.

• Benefit of isotopic dilution method was illustrated for three examples.

Pharmaceuticals and personal care products (PPCPs) are a unique group of emerging and non-persistent contaminants. In this study, 27 PPCPs in various water samples were extracted by solid phase extraction (SPE), and determined by isotope dilution method using liquid chromatography coupled to tandem triple quadruple mass spectrometer (LC-MS/MS). A total of 27 isotopically labeled standards (ILSs) were applied to correct the concentration of PPCPs in spiked ultrapure water, drinking water, river, effluent and influent sewage. The corrected recoveries were 73%–122% with the relative standard deviation (RSD)<16%, except for acetaminophen. The matrix effect for all kinds of water samples was<22% and the method quantitation limits (MQLs) were 0.45–8.6 ng/L. The developed method was successfully applied on environmental water samples. The SPE extracts of spiked ultrapure water, drinking water, river and wastewater effluent were stored for 70 days, and the ILSs-corrected recoveries of 27 PPCPs were obtained to evaluate the correction ability of ILSs in the presence of variety interferences. The recoveries of 27 PPCPs over 70 days were within the scope of 72%–140% with the recovery variation<37% in all cases. The isotope dilution method seems to be of benefit when the extract has to be stored for long time before the instrument analysis.

Keywords Pharmaceuticals and personal care products (PPCPs)      Isotopically labeled standard (ILSs)      Water      Solid-phase extraction (SPE)      LC-MS/MS     
发布日期: 2019-11-08
服务
推荐给朋友
免费邮件订阅
RSS订阅
作者相关文章
Xueqi Fan
Jie Gao
Wenchao Li
Jun Huang
Gang Yu
引用本文:   
Xueqi Fan,Jie Gao,Wenchao Li, et al. Determination of 27 pharmaceuticals and personal care products (PPCPs) in water: The benefit of isotope dilution[J]. Front. Environ. Sci. Eng., 2020, 14(1): 8.
网址:  
https://journal.hep.com.cn/fese/EN/10.1007/s11783-019-1187-3     OR     https://journal.hep.com.cn/fese/EN/Y2020/V14/I1/8
Therapeutic class No. Target
(Abbreviation) (+/-) a)
CAS Precursor
(m/z)
Product
(m/z)
DP b)
(V)
CE c)
(V)
ILS d)
Antihypertensives #1 Propranolol (PPN)+ 3506-09-0 260.3 116.1/56.1 46 25 PPN-D7
Antiepileptic drugs #2 Carbamazepin (CBZ)+ 298-46-4 237.2 194.2/178.9 51 23 CBZ-D10
Vermifuges #3 N,N-diethyl-m-toluamide (DEET)+ 134-62-3 192.3 119.1/91.0 51 23 DEET-D6
Stimulants #4 Caffeine (CF)+ 58-08-2 195.2 138.2/42.1 56 23 CF-D5
Analgesic anti-inflammatory #5 Diclofenac (DF)- 15307-86-5 293.9 249.9/213.9 15 12 DF-D4
#6 Indomethacine (IM)- 53-86-1 356 312.2/297.2 15 10 IM-D4
#7 Mndomethacine (MA)- 61-68-7 239.6 196.0/192.0 35 22 MA-D3
Lipid Regulators #8 Benzafibrate (BF)- 41859-67-0 360 274.0/153.9 30 16 BF-D4
#9 Clofibric acid (CA)- 882-09-7 212.9 126.9/85.0 15 20 CA-D4
Chloramphenicol #10 Chloramphenicol (CP)- 56-75-7 320.9 152.0/256.9 35 26 CP-D5
Tetracyclines #11 Tetracycline (TCN)+ 64-75-5 445.3 410.2/154.4 51 21 TCN-D4
Antipyretic analgesic #12 Acetaminophen (ATP)+ 103-90-2 152.1 110.0/65.1 46 21 ATP-13C,15N
Macrolides #13 Erythromycin (EM)+ 114-07-8 734.4 158.2/576.3 66 37 EM-13C2
#14 Roxithromycin (RXM)+ 80214-83-1 837.6 158.3/558.3 61 43 RXM-D7
Penicillins #15 Penicillin G (PCG)+ 113-98-4 335.2 217.2/91.1 66 17 PCG-D7
Sulfonamides #16 Sulfadiazine (SD)+ 68-35-9 251.1 156.2/92.1 46 19 SD-D4
#17 Sulfathiazole (ST)+ 72-14-0 256.1 156.2/92.0 41 19 ST-D4
#18 Sulfisoxazole (SIX)+ 127-69-5 268.2 156.2/92.0 46 17 SIX-13C6
#19 Sulfamethoxypyridazine
(SMP)+
80-35-3 281.1 156.1/92.0 46 21 SMP-D3
#20 Sulfaquinoxaline (SQX)+ 59-40-5 301.2 156.1/143.1 41 21 SQX-13C6
#21 Sulfamethazine (SMT)+ 57-68-1 279.1 124.2/92.0 51 31 SMT-13C6
#22 Sulfadimethoxine (SDM)+ 122-11-2 311.1 156.2/92.0 61 25 SDM-D4
#23 Sulfamethoxazole (SMX)+ 723-46-6 254.2 156.2/92.0 46 19 SMX-13C6
#24 Sulfamethizol (SMZ)+ 144-82-1 271.1 156.1/92.0 41 17 SMZ-13C6
#25 Sulfamonomethoxine (SM)+ 1220-83-3 281.1 156.2/92.0 46 21 SM-D4
Lincosamides #26 Clindamycin (CDM)+ 58207-19-5 425.2 126.2/377.1 56 39 CDM-D3
#27 Lincomycin (LCM)+ 859-18-7 407.2 126.2/359.1 56 37 LCM-D3
Tab.1  The representative numbers, abbreviations and instrument information of 27 targeted PPCPs
No. PPCPs Ultrapure Drinking Surface Effluent Influent
Recovery (%) RSD
(%)
Recovery (%) RSD (%) Recovery (%) RSD (%) Recovery (%) RSD (%) Recovery (%) RSD (%)
#1 PPN 105 1 104 2 98 2 101 3 102 5
#2 CBZ 113 2 113 3 112 2 122 2 105 2
#3 DEET 114 1 109 1 114 1 122 1 101 10
#4 CF 111 2 104 2 115 3 118 2 102 6
#5 DF 85 5 109 3 110 3 87 1 83 5
#6 IM 105 1 99 1 95 4 80 2 80 8
#7 MA 100 4 106 3 103 4 82 3 74 7
#8 BF 106 3 105 2 106 2 110 4 109 4
#9 CA 114 2 112 1 112 2 114 1 87 4
#10 CP 107 2 105 0 101 2 106 2 108 4
#11 TCN 101 5 103 11 97 11 102 2 110 2
#12 ATP 110 7 116 16 93 34 94 30
#13 EM 106 6 102 6 106 6 114 3 79 10
#14 RXM 89 4 99 2 105 3 97 3 92 6
#15 PCG 109 5 114 4 112 5 101 6 102 7
#16 SD 109 1 117 1 120 3 120 4 116 3
#17 ST 113 2 113 1 112 4 110 2 112 2
#18 SIX 107 3 119 5 120 4 119 2 115 4
#19 SMP 112 3 108 3 108 4 119 3 103 5
#20 SQX 112 2 104 3 109 1 112 3 100 4
#21 SMT 81 7 73 4 79 10 79 8 86 7
#22 SDM 108 3 105 1 111 3 109 4 113 3
#23 SMX 120 3 96 3 99 4 94 5 118 5
#24 SMZ 119 4 119 2 120 3 119 3 110 2
#25 SM 109 4 101 3 101 2 97 4 75 6
#26 CDM 106 2 112 1 112 3 88 2 120 5
#27 LCM 119 5 109 6 120 3 83 6 88 7
Tab.2  The recovery and relative RSD (n = 3) of 27 PPCPs in five kinds of water samples
No. PPCPs Drinking water (n = 2) Surface water (n = 3) WRS-A effluent (n = 3) WRS-A influent (n = 3) WRS-B effluent (n = 3) WRS-B influent (n = 3)
#2 CBZ ND ND 26 76 94 192
#3 DEET ND ND 92 1633 61 481
#4 CF ND 356 39 10334 71 13318
#5 DF ND 9 67 1344 73 489
#6 IM ND ND 19 1260 47 598
#7 MA 2 4 21 431 21 132
#8 BF ND ND ND 65 ND 23
#9 CA ND ND ND 132 ND 12
#10 CP ND ND 5 1365 ND 115
#11 TCN ND ND ND 48 ND 71
#12 ATP ND 20 14 41
#23 SMX ND 6 17 75 15 71
#26 CDM ND ND 36 76 35 79
Tab.3  PPCPs detected in water samples collected in Tsinghua University
Fig.1  The recoveries of 27 PPCPs corrected by 27 ILSs in four kinds of water during 70 days.
Fig.2  The curves 1–4 and curves 5–8 were the recoveries of SMZ for ultrapure water, drinking water, surface water and wastewater effluent corrected by corresponding ILS and non-corresponding ILS over 70 days, respectively.
Fig.3  The curves 1–4 and curves 5–8 were the recoveries of IM for ultrapure water, drinking water, surface water and wastewater effluent corrected by IM-D4 and EM-13C2 over 70 days, respectively.
Fig.4  The curves 1–4 and curves 5–8 were the recoveries of CBZ for ultrapure water, drinking water, surface water and wastewater effluent corrected by CBZ-D10 and PPN-D7 over 70 days, respectively.
1 A M Ali, H T Rønning, L K Sydnes, W M Alarif, R Kallenborn, S S Al-Lihaibi (2018). Detection of PPCPs in marine organisms from contaminated coastal waters of the Saudi Red Sea. Science of the Total Environment, 621: 654–662
https://doi.org/10.1016/j.scitotenv.2017.11.298 pmid: 29197284
2 C Aristizabal-Ciro, A M Botero-Coy, F J López, G A Peñuela (2017). Monitoring pharmaceuticals and personal care products in reservoir water used for drinking water supply. Environmental Science and Pollution Research International, 24(8): 7335–7347
https://doi.org/10.1007/s11356-016-8253-1 pmid: 28105593
3 M Biel-Maeso, C Corada-Fernández, P A Lara-Martín (2019). Removal of personal care products (PCPs) in wastewater and sludge treatment and their occurrence in receiving soils. Water Research, 150: 129–139
https://doi.org/10.1016/j.watres.2018.11.045 pmid: 30508710
4 M Caban, E Lis, J Kumirska, P Stepnowski (2015). Determination of pharmaceutical residues in drinking water in Poland using a new SPE-GC-MS(SIM) method based on Speedisk extraction disks and DIMETRIS derivatization. Science of the Total Environment, 538: 402–411
https://doi.org/10.1016/j.scitotenv.2015.08.076 pmid: 26318224
5 M Q Cai, R Wang, L Feng, L Q Zhang (2015). Determination of selected pharmaceuticals in tap water and drinking water treatment plant by high-performance liquid chromatography-triple quadrupole mass spectrometer in Beijing, China. Environmental Science and Pollution Research International, 22(3): 1854–1867
https://doi.org/10.1007/s11356-014-3473-8 pmid: 25196960
6 F Chen, Z Gong, B C Kelly (2015). Rapid analysis of pharmaceuticals and personal care products in fish plasma micro-aliquots using liquid chromatography tandem mass spectrometry. Journal of Chromatography. A, 1383: 104–111
https://doi.org/10.1016/j.chroma.2015.01.033 pmid: 25640994
7 A Díaz, A Peña-Alvarez (2017). A simple method for the simultaneous determination of pharmaceuticals and personal care products in river sediment by ultrasound-assisted extraction followed by solid-phase microextraction coupled with gas chromatography-mass spectrometry. Journal of Chromatographic Science, 55(9): 946–953
https://doi.org/10.1093/chromsci/bmx058 pmid: 29048490
8 B Du, P Perez-Hurtado, B W Brooks, C K Chambliss (2012). Evaluation of an isotope dilution liquid chromatography tandem mass spectrometry method for pharmaceuticals in fish. Journal of Chromatography. A, 1253: 177–183
https://doi.org/10.1016/j.chroma.2012.07.026 pmid: 22840821
9 A J Ebele, M A Abdallah, S Harrad (2017). Pharmaceuticals and personal care products (PPCPs) in the freshwater aquatic environment. Emerging Contaminants, 3(1): 1–16
https://doi.org/10.1016/j.emcon.2016.12.004
10 X Fan, S Zhao, J Hu (2019). Dissipation behavior and dietary risk assessment of lambda-cyhalothrin, thiamethoxam and its metabolite clothianidin in apple after open field application. Regulatory Toxicology and Pharmacology, 101: 135–141
https://doi.org/10.1016/j.yrtph.2018.11.003 pmid: 30445137
11 M J Gómez, M J Martínez Bueno, S Lacorte, A R Fernández-Alba, A Agüera (2007). Pilot survey monitoring pharmaceuticals and related compounds in a sewage treatment plant located on the Mediterranean coast. Chemosphere, 66(6): 993–1002
https://doi.org/10.1016/j.chemosphere.2006.07.051 pmid: 16962638
12 C Hao, X Zhao, P Yang (2007). GC-MS and HPLC-MS analysis of bioactive pharmaceuticals and personal care products in environmental matrices. Trends in Analytical Chemistry, 26(6): 569–580
https://doi.org/10.1016/j.trac.2007.02.011
13 H Huang, J Wu, J Ye, T Ye, J Deng, Y Liang, W Liu (2018). Occurrence, removal, and environmental risks of pharmaceuticals in wastewater treatment plants in south China. Frontiers of Environmental Science & Engineering 12(6): 7
https://doi.org/10.1007/s11783-018-1053-8
14 X Jiang, Y Qu, L Liu, Y He, W Li, J Huang, H Yang, G Yu (2019). PPCPs in a drinking water treatment plant in the Yangtze River Delta of China: Occurrence, removal and risk assessment. Frontiers of Environmental Science & Engineering, 13(2): 27
https://doi.org/10.1007/s11783-019-1109-4
15 J J Jiménez, M I Sánchez, R Pardo, B E Muñoz (2017). Degradation of indomethacin in river water under stress and non-stress laboratory conditions: degradation products, long-term evolution and adsorption to sediment. Journal of environmental sciences-China, 51: 13–20 S1001074216306143
pmid: 28115123
16 T Lin, S Yu, W Chen (2016). Occurrence, removal and risk assessment of pharmaceutical and personal care products (PPCPs) in an advanced drinking water treatment plant (ADWTP) around Taihu Lake in China. Chemosphere, 152: 1–9
https://doi.org/10.1016/j.chemosphere.2016.02.109 pmid: 26943873
17 D Löffler, J Römbke, M Meller, T A Ternes (2005). Environmental fate of pharmaceuticals in water/sediment systems. Environmental Science & Technology, 39(14): 5209–5218
https://doi.org/10.1021/es0484146 pmid: 16082949
18 S C Monteiro, A B Boxall (2009). Factors affecting the degradation of pharmaceuticals in agricultural soils. Environmental Toxicology and Chemistry, 28(12): 2546–2554
https://doi.org/10.1897/08-657.1 pmid: 19580336
19 T S Oliveira, M Murphy, N Mendola, V Wong, D Carlson, L Waring (2015). Characterization of pharmaceuticals and personal care products in hospital effluent and waste water influent/effluent by direct-injection LC-MS-MS. Science of the Total Environment, 518–519: 459–478
20 M Papageorgiou, C Kosma, D Lambropoulou (2016). Seasonal occurrence, removal, mass loading and environmental risk assessment of 55 pharmaceuticals and personal care products in a municipal wastewater treatment plant in Central Greece. Science of the Total Environment, 543(Pt A): 547–569
https://doi.org/10.1016/j.scitotenv.2015.11.047 pmid: 26613513
21 B Petrie, E J McAdam, M D Scrimshaw, J N Lester, E Cartmell (2013). Fate of drugs during wastewater treatment. Trends in Analytical Chemistry, 49(49): 145–159
https://doi.org/10.1016/j.trac.2013.05.007
22 E G Primel, S S Caldas, A L Escarrone (2012). Multi-residue analytical methods for the determination of pesticides and PPCPs in water by LC-MS/MS: A review. Central European Journal of Chemistry, 10(3): 876–899
23 J A Rivera-Jaimes, C Postigo, R M Melgoza-Alemán, J Aceña, D Barceló, M López de Alda (2018). Study of pharmaceuticals in surface and wastewater from Cuernavaca, Morelos, Mexico: Occurrence and environmental risk assessment. Science of the Total Environment, 613–614: 1263–1274
https://doi.org/10.1016/j.scitotenv.2017.09.134 pmid: 28962074
24 Q Sui, J Huang, S Deng, G Yu, Q Fan (2010). Occurrence and removal of pharmaceuticals, caffeine and DEET in wastewater treatment plants of Beijing, China. Water Research, 44(2): 417–426
https://doi.org/10.1016/j.watres.2009.07.010 pmid: 19674764
25 R Tanoue, K Nomiyama, H Nakamura, T Hayashi, J W Kim, T Isobe, R Shinohara, S Tanabe (2014). Simultaneous determination of polar pharmaceuticals and personal care products in biological organs and tissues. Journal of Chromatography. A, 1355: 193–205
https://doi.org/10.1016/j.chroma.2014.06.016 pmid: 24958034
26 N H Tran, J Hu, S L Ong (2013). Simultaneous determination of PPCPs, EDCs, and artificial sweeteners in environmental water samples using a single-step SPE coupled with HPLC-MS/MS and isotope dilution. Talanta, 113(17): 82–92
https://doi.org/10.1016/j.talanta.2013.03.072 pmid: 23708627
27 N H Tran, J Li, J Hu, S L Ong (2014). Occurrence and suitability of pharmaceuticals and personal care products as molecular markers for raw wastewater contamination in surface water and groundwater. Environmental Science and Pollution Research International, 21(6): 4727–4740
https://doi.org/10.1007/s11356-013-2428-9 pmid: 24352549
28 USEPA (2007). Method 1694: Pharmaceuticals and Personal Care Products in Water, Soil, Sediment, and Biosolids by HPLC/MS/MS. Washington, DC: US Environmental Protection Agency
29 J Wang, S Wang (2016). Removal of pharmaceuticals and personal care products (PPCPs) from wastewater: A review. Journal of Environmental Management, 182: 620–640
https://doi.org/10.1016/j.jenvman.2016.07.049 pmid: 27552641
30 Y Yang, S O Yong, K H Kim, E E Kwon, Y F Tsang (2017). Occurrences and removal of pharmaceuticals and personal care products (PPCPs) in drinking water and water/sewage treatment plants: A review. Science of the Total Environment, 596–597: 303–320
31 Y Zhang, W Guo, Z Yue, L Lin, F Zhao, P Chen, W Wu, H Zhu, B Yang, Y Kuang, J Wang (2017). Rapid determination of 54 pharmaceutical and personal care products in fish samples using microwave-assisted extraction-Hollow fiber-Liquid/solid phase microextraction. Journal of Chromatography. B, Analytical Technologies in the Biomedical and Life Sciences, 1051: 41–53
https://doi.org/10.1016/j.jchromb.2017.01.026 pmid: 28292733
[1] FSE-19083-OF-FXQ_suppl_1 Download
No related articles found!
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed   
版权所有 © 2015 高等教育出版社.
电话: 010-58556848 (技术); 010-58556485 (订阅) E-mail: subscribe@hep.com.cn