Spatiotemporal differential distribution characteristics and ecological risk assessment of antibiotics in the Yangtze River Estuary and offshore areas

doi:10.3969/j.issn.1000-5641.2024.06.012

Abstract

Abstract:

As the ultimate destination of antibiotics in rivers, the mechanism and change law of migration from rivers to oceans have not been fully and systematically studied. In this study, surface water samples were collected in the Yangtze River Estuary and its offshore areas in the wet season and dry season of 2023. Solid-phase extraction and high performance liquid chromatography-mass spectrometry were used to identify 20 antibiotics in five categories. This analysis was conducted to assess the concentrations, temporal and spatial distribution, and potential ecological risks. The results showed that the concentrations of 20 antibiotics ranged from not detected ~ 63.32 ng·L^–1, and showed a decreasing trend from inland to marine areas from the mouth-adjacent section (average 108 ng·L^–1) to the estuary section (average 50 ng·L^–1), to the coastal section outside the mouth (average 40 ng·L^–1), and the coastal area (average 29 ng·L^–1). The concentrations of the five types of antibiotics from high to low were chloramphenicols > macrolides > sulfonamides > quinolones > tetracyclines. The categories and amount of detected antibiotics showed significant seasonal differences. The seasonal-change pattern showed that the ML concentration season was significantly higher in the dry than the wet season, while the concentrations of TCs were significantly higher in the wet season than the dry season. Antibiotics, such as Sulfamethoxazole, Ciprofloxacin, Chlortetracycline, Erythromycin, Chloramphenicol, Ofloxacin, posed a significant threat to the water in the study area, and the ecological risks should not be overlooked.

Key words: antibiotics, Yangtze River Estuary, offshore areas, temporal and spatial distribution, ecological risk

CLC Number:

X826

Yuyi WANG, Ye HUANG, Jing YANG, Fangfang DING, Tianhao HE, Yushan LI, Lin HUANG, Ye LI, Min LIU. Spatiotemporal differential distribution characteristics and ecological risk assessment of antibiotics in the Yangtze River Estuary and offshore areas[J]. Journal of East China Normal University(Natural Science), 2024, 2024(6): 136-150.

Figures/Tables 10

Fig.1

Table 1

Table 2

Table 3

Ecotoxic parameters of target compounds"

抗生素	物种类别	受试物种	效应类型	毒性数据/(mg·L^–1)	评估因子	C_PNE/(ng·L^–1)	参考文献
SP	Algae	M. macrocopa	L (E) C₅₀	1.2	1000	1200	[24]
	Daphnia	D. magna	L (E) C₅₀	149.3	1000	149300	[25]
	Fish	O. latipes	L (E) C₅₀	> 500	1000	500000	[25]
SDZ	Algae	C. vulgaris.	L (E) C₅₀	1.226	1000	1226	[26]
	Daphnia	D. magna	L (E) C₅₀	212	1000	212000	[27]
	Fish	-	L (E) C₅₀	50.29	1000	50290	[28]
SMX	Algae	S. leopoliensis	L (E) C₅₀	0.027	1000	27	[29]
	Daphnia	C. dubia	L (E) C₅₀	0.21	1000	210	[30]
	Fish	O. latipes	L (E) C₅₀	562.5	1000	562500	[31]
ST	Algae	S. leopoliensis	L (E) C₅₀	13.1	100	13100	[32]
	Daphnia	D. magna	L (E) C₅₀	17	100	17000	[32]
	Fish	O. latipes	L (E) C₅₀	500	100	500000	[32]
SMR	Algae	S. vacuolatus	L (E) C₅₀	11.9	1000	11900	[33]
	Daphnia	D. magna	L (E) C₅₀	66.22	1000	66220	[34]
	Fish	-	L (E) C₅₀	100	1000	100000	[35]
SMZ	Algae	P. subcapitata	NOEC	0.001	100	10000	[36]
	Daphnia	D. magna	L (E) C₅₀	158.8	1000	158800	[31]
	Fish	O. latipes	L (E) C₅₀	> 100	1000	100000	[31]
SQ	Algae	P. subcapitata	L (E) C₅₀	0.246	1000	246	[32]
	Daphnia	D. magna	L (E) C₅₀	131	1000	131000	[32]
	Fish	O. latipes	L (E) C₅₀	234.8	1000	234800	[32]
NFX	Algae	M. wesenbergii	L (E) C₅₀	0.038	1000	38	[32]
	Daphnia	Daphnid	L (E) C₅₀	1800	1000	3093133	[32]
	Fish	P. olivaceus	L (E) C₅₀	100	1000	100000	ECOTOX
CIP	Algae	M. aeruginosa	L (E) C₅₀	0.005	1000	5	[37]
	Daphnia	D. magna	L (E) C₅₀	1.58726	1000	1587	ECOTOX
	Fish	G. holbrooki	L (E) C₅₀	60	1000	60000	ECOTOX
EFX	Algae	M. aeruginosa	L (E) C₅₀	0.049	1000	49	[38]
	Daphnia	D. magna	L (E) C₅₀	56.7	1000	56700	[25]
	Fish	O. latipes	L (E) C₅₀	> 100	1000	100000	[25]
OFX	Algae	S. leopoliensis	L (E) C₅₀	0.016	1000	16	[30]
	Daphnia	C. dubia	L (E) C₅₀	3.13	1000	3130	[30]
	Fish	D. rerio	L (E) C₅₀	> 1000	1000	1000	[37]
TC	Algae	M. aeruginosa	L (E) C₅₀	0.05	1000	50	[39]
	Daphnia	D. magna	L (E) C₅₀	36.56	1000	36560	[34]
	Fish	G. holbrooki	NOEC	5	100	50000	[40]
DC	Algae	G. algae	L (E) C₅₀	0.32	1000	320	[41]
	Daphnia	C. dubia	L (E) C₅₀	0.5	1000	500	[41]
	Fish	D. rerio	L (E) C₅₀	2.658	1000	2658	[42]
OTC	Algae	P. subcapitata	L (E) C₅₀	0.17	1000	170	[30]
	Daphnia	D. magna	L (E) C₅₀	427.12	1000	427120	[30]
	Fish	S. aurata	NOEC	8	100	80000	[43]
CTC	Algae	P. subcapitata	L (E) C₅₀	0.002	1000	2	[44]
	Daphnia	D. magna	L (E) C₅₀	0.05	1000	88000	[45]
	Fish	Danio rerio	L (E) C₅₀	36.56	1000	12	[46]
ETM	Algae	-	L (E) C₅₀	0.02	1000	20	[30]
	Daphnia	C. dubia	L (E) C₅₀	0.22	1000	220	[47]
	Fish	-	L (E) C₅₀	61	1000	61000	[48]
RTM	Algae	P. subcapitata	L (E) C₅₀	0.01	100	100	[36]
	Daphnia	D. magna	L (E) C₅₀	7.1	100	71000	[49]
	Fish	O. latipes	L (E) C₅₀	50.3	100	503000	[49]
FF	Algae	P. subcapitata	L (E) C₅₀	2.3	1000	2300	[37]
	Daphnia	D. magna	L (E) C₅₀	1.9	1000	1600	[50]
	Fish	O. mossambicus	L (E) C₅₀	50	1000	50000	[51]
TAP	Algae	M. aeruginosa	L (E) C₅₀	0.32	1000	320	[30]
	Daphnia	Daphnid	L (E) C₅₀	8100	1000	8100000	ECOTOX
	Fish	-	L (E) C₅₀	12248	1000	12248000	ECOTOX
CAP	Algae	D. subspicatus	L (E) C₅₀	0.13	1000	130	[52]
	Daphnia	Daphnid	L (E) C₅₀	72.1	1000	72100	ECOTOX
	Fish	-	L (E) C₅₀	38.8	1000	38800	ECOTOX

Table 3

Table 4

Fig.2

Fig.3

Fig.4

Fig.5

Fig.6

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萃取过程	溶剂	流速/ (mL·min^–1)	体积/mL
活化	甲醇	1	10
活化	超纯水	1	10
活化	超纯水 (pH值为5)	1	10
富集		5	1000
清洗杂质	超纯水	1	10
吹干
洗脱	甲醇-乙腈 (1:1)	1	10
旋蒸			0.5
置换	甲醇		8
旋蒸			0.5

种类	名称	英文名称	简称	分子式	CAS号
磺胺类 SAs (sulfonamides)	磺胺吡啶	sulfapyridine	SP	C₁₁H₁₁N₃O₂S	144-83-2
	磺胺嘧啶	sulfadiazine	SDZ	C₁₀H₁₀N₄O₂S	68-35-9
	磺胺甲恶唑	sulfamethoxazole	SMX	C₁₀H₁₁N₃O₃S	723-46-6
	磺胺噻唑	sulfathiazole	ST	C₉H₉N₃O₂S₂	72-14-0
	磺胺间甲基嘧啶	sulfamerazine	SMR	C₁₁H₁₂N₄O₂S	127-79-7
	磺胺二甲(基)嘧啶	sulfamethazine	SMZ	C₁₂H₁₄N₄O₂S	57-68-1
	磺胺喹恶啉	sulfaquinoxaline	SQ	C₁₄H₁₂N₄O₂S	59-40-5
喹诺酮类 QNs (quinolones)	诺氟沙星	norfluxacin	NFX	C₁₆H₁₈FN₃O₃	70458-96-7
	环丙沙星	ciprofloxacin	CIP	C₁₇H₁₈FN₃O₃	85721-33-1
	恩诺沙星	enrofloxacin	EFX	C₁₉H₂₂FN₃O₃	93106-60-6
	氧氟沙星	ofloxacin	OFX	C₁₈H₂₀FN₃O₄	82419-36-1
四环素类 TCs (tetracyclines)	四环素	tetracycline	TC	C₂₂H₂₄N₂O₈	60-54-8
	强力霉素	doxycycline	DC	C₂₂H₂₄N₂O₈	564-25-0
	土霉素	oxytetracycline	OTC	C₂₂H₂₄N₂O₉	79-57-2
	金霉素	chlortetracycline	CTC	C₂₂H₂₃ClN₂O₈	57-62-5
大环内酯类 MLs (macrolides)	红霉素	erythromycin	ETM	C₃₇H₆₇NO₁₃	114-07-8
大环内酯类 MLs (macrolides)	罗红霉素	roxithromycin	RTM	C₄₁H₇₆N₂O₁₅	80214-83-1
氯霉素类 CPs (chloramphenicols)	氟苯尼考	florfenicol	FF	C₁₂H₁₄Cl₂FNO₄S	73231-34-2
	甲砜霉素	thiamphenicol	TAP	C₁₂H₁₅C_l2NO₅S	15318-45-3
	氯霉素	chloramphenicol	CAP	C₁₁H₁₂Cl₂N₂O₅	56-75-7

抗生素	范围/(ng·L^–1)	平均值/(ng·L^–1)	检出率	标准差	范围/(ng·L^–1)	平均值/(ng·L^–1)	检出率	标准差
抗生素	枯水期				丰水期
SMR	0.03 ~ 0.75	0.07	100%	0.13	0.23 ~ 12.25	0.75	100%	1.89
SMZ	ND ~ 5.41	0.64	50.00%	1.83	0.07 ~ 4.75	1.16	100%	1.07
SMX	0.18 ~ 19.29	5.00	100%	6.00	0.35 ~ 23.81	7.17	100%	7.18
SP	0.01 ~ 3.67	0.44	97.06%	0.76	0.15 ~ 1.80	0.66	100%	0.53
ST	ND ~ 1.37	0.22	88.23%	0.40	0.11 ~ 0.48	0.26	100%	0.08
SQ	ND ~ 0.15	0.01	26.47%	0.04	ND ~ 2.52	0.53	67.65%	0.55
SDZ	ND ~ 3.35	0.57	100%	0.83	ND ~ 0.75	0.26	94.12%	0.18
SAs	0.52 ~ 29.26	6.95	-	8.86	1.35 ~ 24.53	7.92	-	9.89
EFX	ND ~ 4.13	0.18	38.23%	1.12	0.25 ~ 5.29	1.11	100%	1.01
OFX	ND ~ 1.72	0.50	94.12%	0.44	0.27 ~ 4.56	1.35	100%	1.14
NFX	ND ~ 8.39	0.96	94.12%	1.46	ND ~ 3.50	0.67	97.06%	0.65
CIP	ND ~ 2.64	0.63	91.18%	0.54	0.22 ~ 8.21	1.62	100%	1.53
QNs	0.58 ~ 15.84	2.27	-	2.73	1.09 ~ 13.86	4.03	-	3.62
CTC	0.30 ~ 1.74	0.45	97.06%	0.19	ND ~ 63.32	8.71	97.06%	16.77
DC	0.30 ~ 0.50	0.40	97.06%	0.02	0.63 ~ 16.08	2.16	100%	2.94
TC	0.32 ~ 1.55	0.43	97.06%	0.15	0.02 ~ 1.96	0.66	100%	0.42
OTC	0.31 ~ 0.66	0.41	70.59%	0.04	1.43 ~ 16.21	4.98	100%	3.40
TCs	1.32 ~ 4.34	1.69	-	0.58	3.94 ~ 68.32	12.47	-	19.26
ETM	0 ~ 37.79	2.38	58.82%	8.17	0.73 ~ 4.73	1.98	100%	1.01
RTM	0.17 ~ 4.32	0.44	100%	0.75	0.02 ~ 1.10	0.20	100%	0.24
MLs	0.17 ~ 42.10	2.82	-	7.22	0.92 ~ 4.74	2.17	-	0.98
CAP	ND ~ 3.71	0.54	41.18%	1.23	0.32 ~ 33.36	8.15	100%	10.58
FF	ND ~ 56.28	11.93	73.53%	20.83	0.12 ~ 5.91	1.83	100%	1.56
TAP	ND ~ 16.83	2.29	52.94%	5.85	ND ~ 9.13	1.38	97.06%	1.65
CPs	ND ~ 76.82	14.76	-	24.09	0.61 ~ 39.02	7.23	-	12.66

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