中国典型红树林沉积物中多溴联苯醚和替代型溴系阻燃剂污染特征

doi:10.11978/2021003

热带海洋学报 ›› 2022, Vol. 41 ›› Issue (1): 117-130.doi: 10.11978/2021003CSTR: 32234.14.2021003

中国典型红树林沉积物中多溴联苯醚和替代型溴系阻燃剂污染特征

李华薇^1,⁴(), 徐向荣^1,^2,³()

1. 中国科学院热带海洋生物资源与生态重点实验室, 中国科学院南海海洋研究所, 广东广州 510301
2. 中国科学院南海生态环境工程创新研究院, 广东广州 510301
3. 南方海洋科学与工程广东省实验室(广州), 广东广州 511458
4. 中国科学院大学, 北京 100049

收稿日期:2021-01-04 修回日期:2021-03-11 出版日期:2022-01-10 发布日期:2022-01-26
通讯作者: 徐向荣
作者简介:李华薇(1994—), 女, 江西省九江市人, 博士研究生, 从事持久性有机污染物的生物地球化学行为研究。email: soledadlee1227@163.com
基金资助:
国家重点研发项目(2018YFC1406503);中国科学院南海生态环境工程创新研究院自主部署项目(ISEE2019ZR03);中国科学院南海生态环境工程创新研究院自主部署项目(ISEE2018PY03);中国科学院南海生态环境工程创新研究院自主部署项目(ISEE2018ZD02);南方海洋科学与工程广东省实验室(广州)人才团队引进重大专项(GML2019ZD0404)

Pollution characteristics of polybrominated diphenyl ethers and alternative brominated flame retardants in sediments from typical mangrove wetlands of China

LI Huawei^1,⁴(), XU Xiangrong^1,^2,³()

1. Key Laboratory of Tropical Marine Bio-resources and Ecology, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China
2. Innovation Academy of South China Sea Ecology and Environmental Engineering, Chinese Academy of Sciences, Guangzhou 510301, China
3. Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou), Guangzhou 511458, China
4. University of Chinese Academy of Sciences, Beijing 100049, China

Received:2021-01-04 Revised:2021-03-11 Online:2022-01-10 Published:2022-01-26
Contact: XU Xiangrong
Supported by:
National Key Research and Development Program of China(2018YFC1406503);Innovation Academy of South China Sea Ecology and Environmental Engineering, Chinese Academy of Sciences(ISEE2019ZR03);Innovation Academy of South China Sea Ecology and Environmental Engineering, Chinese Academy of Sciences(ISEE2018PY03);Innovation Academy of South China Sea Ecology and Environmental Engineering, Chinese Academy of Sciences(ISEE2018ZD02);Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering, Guangdong Laboratory (Guangzhou)(GML2019ZD0404)

摘要/Abstract

摘要：

本文研究了中国四省区(福建、广东、广西和海南)共16处红树林湿地表层沉积物中多溴联苯醚(polybrominated diphenyl ethers, PBDEs)和5种替代型溴系阻燃剂(alternative brominated flame retardants, ABFRs)的污染特征, 包括十溴二苯乙烷(decabromodiphenyl ethane, DBDPE)、1, 2-双(2, 4, 6-三溴苯氧基)乙烷[1, 2-bis (2, 4, 6-tribromophenoxy) ethane, BTBPE]、六溴苯(hexabromobenzene, HBB)、五溴甲苯(pentabromotoluene, PBT)和五溴乙苯(pentabromoethylbenzene, PBEB)。结果表明, PBDEs、DBDPE和BTBPE在我国红树林湿地沉积物中广泛存在, 而HBB、PBT和PBEB仅在部分红树林湿地检出。PBDEs总含量的均值范围为1.39~293ng·g^-1(干重), 其污染程度具有明显的空间差异性(p=0.016), 并且与当地人口和经济水平显著正相关(p<0.01)。在红树林沉积物样品中, BDE 209是最主要的同系物, 占PBDEs总含量的72%~96%; DBDPE和BTBPE是最主要的ABFRs, 浓度的均值范围分别为0.489~29.4ng·g^-1(干重)和0.0127~1.11ng·g^-1(干重)。BDE 209与其替代品DBDPE的含量显著正相关(p<0.01), 反映出二者在红树林湿地沉积物中空间分布的相似性, 这说明BDE 209和DBDPE可能具有相似的污染源和/或环境行为。DBDPE与BDE 209的浓度比值范围为0.0839~0.925, 表明我国红树林湿地沉积物中DBDPE的污染水平还未超过BDE 209, 但ABFRs逐渐替代使用而带来的环境问题不容忽视。

关键词: 红树林, 多溴联苯醚, 替代型溴系阻燃剂, 沉积物, 空间分布

Abstract:

Surface sediment samples were collected from 16 mangrove wetlands in four provinces (Fujian, Guangdong, Guangxi and Hainan) of China and analyzed for polybrominated diphenyl ethers (PBDEs) and five alternative brominated flame retardants (ABFRs), including decabromodiphenyl ethane (DBDPE), 1, 2-bis (2, 4, 6-tribromophenoxy) ethane (BTBPE), hexabromobenzene (HBB), pentabromotoluene (PBT) and pentabromoethylbenzene (PBEB). Results showed that PBDEs, DBDPE and BTBPE were widely detected in the mangrove sediments, while HBB, PBT and PBEB were only observed in some regions. Average concentrations of total PBDEs ranged from 1.39 to 293 ng·g^-1dry weight (dw), showing an obvious spatial difference (p=0.016), which was significantly positively correlated with the local population and economic levels (p<0.01). BDE 209 was the predominant congener in all mangrove sediments, accounting for 72%~96% of the total PBDEs. DBDPE and BTBPE were the two dominant ABFRs, with average concentrations ranging from 0.489 to 29.4 ng·g^-1 and from 0.0127 to 1.11 ng·g^-1, respectively. There was a significant positive relationship between levels of BDE 209 and its alternative, DBDPE (p<0.01), reflecting their similar regional distributions in the mangrove sediments. This suggests that BDE 209 and DBDPE might have similar pollution resources and/or environmental behaviors. Ratios of DBDPE/BDE 209 were in the range of 0.0839~0.925, which indicates that levels of DBDPE were still lower than those of BDE 209 in the mangrove sediments of China. Still, environmental issues of ABFRs should not be ignored.

Key words: mangrove, polybrominated diphenyl ethers, alternative brominated flame retardants, sediment, spatial distribution

中图分类号:

P734.5

李华薇, 徐向荣. 中国典型红树林沉积物中多溴联苯醚和替代型溴系阻燃剂污染特征[J]. 热带海洋学报, 2022, 41(1): 117-130.

LI Huawei, XU Xiangrong. Pollution characteristics of polybrominated diphenyl ethers and alternative brominated flame retardants in sediments from typical mangrove wetlands of China[J]. Journal of Tropical Oceanography, 2022, 41(1): 117-130.

图/表 14

表1

红树林沉积物样品采集信息表"

采样点		样品数	经度范围	纬度范围	所属红树林或保护区
福建	福鼎	5	120°11′43″—120°22′32″E	27°13′23″—27°16′47″N	姚家屿红树林自然保护区
	泉州	3	118°41′2″—118°41′53″E	24°54′41″—24°57′27″N	泉州湾红树林省级自然保护区
	龙海	7	117°53′27″—117°56′44″E	24°23′38″—24°28′11″N	九龙江口红树林省级自然保护区
	漳江口	5	117°23′7″—117°27′37″E	21°54′41″—23°56′15″N	漳江口红树林国家级自然保护区
广东	深圳	7	114°0′19″—114°0′51″E	22°31′24″—22°31′40″N	内伶仃岛-福田国家级自然保护区
	广州	12	113°34′38″—113°34′44″E	22°48′46″—22°48′50″N	南沙区坦头红树林
	珠海	13	113°37′37″—113°38′00″E	22°25′36″—22°25′59″N	淇澳-担杆岛省级自然保护区
广西	山口	6	109°40′13″—109°45′32″E	21°30′12″—21°36′4″N	山口红树林国家级自然保护区
	北海	3	109°6′15″—109°9′18″E	21°33′33″—21°53′13″N	廉州湾南流江入海口处红树林
	钦州	7	108°29′41″—108°37′17″E	21°44′34″—21°53′13″N	茅尾海红树林省级自然保护区
	防城港	4	108°19′41″—108°25′2″E	21°36′47″—21°40′58″N	港口区渔洲坪红树林
	北仑河口	5	108°9′25″—108°16′1″E	21°32′56″—21°36′56″N	北仑河口国家级自然保护区
海南	花场	4	109°59′30″—109°59′52″E	19°54′43″—19°55′7″N	花场湾红树林自然保护区
	文昌	5	110°47′15″—110°50′27″E	19°33′27″—19°37′32″N	清澜港红树林省级自然保护区
	三亚	5	109°30′27″—109°37′18″E	18°13′42″—18°16′18″N	青梅港和三亚河红树林自然保护区
	东方	4	108°37′55″—108°38′15″E	19°12′55″—19°13′1″N	东方市四必湾湿地

表1

表2

红树林沉积物中PBDEs的浓度/(ng·g-1 干重)"

采样点	BDE 28	BDE 47	BDE 66	BDE 99	BDE 100	BDE 153	BDE 154	BDE 183	BDE 196	BDE 197	BDE 202	BDE 203	BDE 206	BDE 207	BDE 208	BDE 209	∑PBDEs^a
福建省
福鼎	0.00207 ± 0.000288^b	0.123 ± 0.0202	0.0172 ± 0.00283	nd^c	nd	0.00466 ± 0.000544	0.00879 ± 0.00139	0.0978 ± 0.0157	0.117 ± 0.0145	0.0361 ± 0.00453	0.0271 ± 0.00419	0.0466 ± 0.00890	0.230 ± 0.0176	0.0829 ± 0.0108	0.0315 ± 0.00571	9.90 ± 1.76	10.7 ± 1.79
泉州	0.00363 ± 0.000477	0.526 ± 0.205	0.0211 ± 0.00366	nd	nd	0.00695 ± 0.000207	nd	0.0373 ± 0.00613	0.108 ± 0.00891	0.0329 ± 0.00659	0.0278 ± 0.00736	0.0462 ± 0.00161	0.221 ± 0.0112	0.0735 ± 0.0103	0.0267 ± 0.00139	12.4 ± 0.987	13.6 ± 1.22
龙海	0.00381 ± 0.000260	0.579 ± 0.176	0.0176 ± 0.00360	0.0134 ± 0.00407	0.00360 ± 0.000552	0.00558 ± 0.000366	0.00706 ± 0.00113	0.0498 ± 0.00666	0.138 ± 0.0309	0.0495 ± 0.00848	0.0334 ± 0.00593	0.0737 ± 0.0223	0.603 ± 0.198	0.258 ± 0.101	0.170 ± 0.0590	30.9 ± 6.22	32.9 ± 6.64
漳江口	0.00286 ± 0.000338	0.118 ± 0.0342	0.00759 ± 0.00213	nd	0.00531 ± 0.000586	0.00489 ± 0.000311	nd	0.0527 ± 0.00738	0.0932 ± 0.00971	0.0443 ± 0.0115	0.0381 ± 0.00779	0.0382 ± 0.00579	0.221 ± 0.0705	0.0491 ± 0.0283	0.0260 ± 0.00983	13.7 ± 5.93	14.4 ± 6.08
广东省
深圳	0.0140 ± 0.00463	0.145 ± 0.0608	0.0126 ± 0.00411	0.0459 ± 0.00661	0.0135 ± 0.00128	0.00823 ± 0.00281	nd	0.289 ± 0.104	0.262 ± 0.0351	0.176 ± 0.0499	0.128 ± 0.00531	0.174 ± 0.0243	1.34 ± 0.132	0.682 ± 0.0810	0.419 ± 0.0425	94.7 ± 6.33	98.4 ± 6.62
广州	0.0102 ± 0.000931	4.26 ± 2.64	0.00710 ± 0.000681	0.555 ± 0.273	0.0900 ± 0.0424	0.292 ± 0.122	0.242 ± 0.110	0.734 ± 0.263	2.93 ± 1.65	0.999 ± 0.514	0.367 ± 0.154	2.04 ± 1.12	12.0 ± 6.81	6.31 ± 3.53	3.82 ± 2.32	258 ± 104	293 ± 122
珠海	0.00494 ± 0.000676	0.235 ± 0.0725	0.00575 ± 0.000519	0.0204 ± 0.00303	0.00591 ± 0.000885	0.00564 ± 0.000332	0.0158 ± 0.00269	0.0676 ± 0.00535	0.129 ± 0.0262	0.0507 ± 0.00846	0.0497 ± 0.0148	0.0746 ± 0.0198	0.412 ± 0.135	0.179 ± 0.0611	0.126 ± 0.0501	17.9 ± 3.50	19.2 ± 3.81
广西壮族自治区
山口	0.00382 ± 0.000680	0.174 ± 0.0857	0.0127 ± 0.00566	nd	nd	0.00368 ± 0.0000972	nd	0.0822 ± 0.0179	0.0811 ± 0.00534	0.0247 ± 0.00179	0.0266 ± 0.00317	0.0362 ± 0.00258	0.0980 ± 0.00658	0.0170 ± 0.00497	0.0147 ± 0.00181	2.77 ± 0.495	3.32 ± 0.500
北海	0.00309 ± 0.000464	0.131 ± 0.0807	0.00488 ± 0.000675	nd	nd	0.00388 ± 0.000383	nd	0.0751 ± 0.0393	0.237 ± 0.150	0.0227 ± 0.00566	0.0838 ± 0.0696	0.0420 ± 0.0121	0.285 ± 0.142	0.115 ± 0.0814	0.0534 ± 0.0387	11.8 ± 6.15	12.8 ± 6.62
钦州	0.00296 ± 0.000417	0.265 ± 0.0745	0.00456 ± 0.00107	nd	0.00451 ± 0.00119	0.00488 ± 0.000732	0.0154 ± 0.00499	0.0734 ± 0.0334	0.288 ± 0.192	0.101 ± 0.0695	0.0371 ± 0.0158	0.218 ± 0.161	1.47 ± 1.22	0.892 ± 0.802	0.475 ± 0.428	34.7 ± 16.5	38.5 ± 19.4
防城港	0.00608 ± 0.00152	0.218 ± 0.180	0.00587 ± 0.00130	nd	nd	0.00397 ± 0.000495	nd	0.0636 ± 0.0216	0.0830 ± 0.00471	0.0313 ± 0.00424	0.0227 ± 0.00521	0.0380 ± 0.00486	0.145 ± 0.0410	0.0462 ± 0.0225	0.0290 ± 0.00865	6.40 ± 2.91	7.10 ± 3.14
北仑河口	0.0105 ± 0.00484	0.0273 ± 0.00748	0.0151 ± 0.00518	nd	nd	0.00383 ± 0.000192	nd	0.0832 ± 0.0196	0.0790 ± 0.00291	0.0425 ± 0.00956	0.0151 ± 0.00317	0.0372 ± 0.00542	0.101 ± 0.00877	0.0114 ± 0.00136	0.0160 ± 0.00498	2.13 ± 0.820	2.54 ± 0.868
海南省
花场	0.00402 ± 0.00104	0.0362 ± 0.00734	0.00833 ± 0.00262	nd	nd	0.00387 ± 0.000114	nd	0.0778 ± 0.00741	0.0737 ± 0.00194	0.0301 ± 0.00445	0.0204 ± 0.00483	0.0290 ± 0.00215	0.0908 ± 0.00409	0.0104 ± 0.00113	0.0170 ± 0.00171	1.00 ± 0.0704	1.39 ± 0.0719
文昌	0.00670 ± 0.00180	0.0911 ± 0.0318	0.00742 ± 0.00332	nd	nd	0.00717 ± 0.00185	nd	0.0628 ± 0.0208	0.117 ± 0.0115	0.0571 ± 0.0245	0.0503 ± 0.0228	0.0793 ± 0.0241	0.196 ± 0.0587	0.0853 ± 0.0506	0.0714 ± 0.0328	4.18 ± 2.28	4.98 ± 2.49
三亚	0.160 ± 0.121	0.262 ± 0.155	0.0359 ± 0.0307	nd	nd	0.00765 ± 0.00174	nd	0.0774 ± 0.0546	0.181 ± 0.0467	0.107 ± 0.0532	0.113 ± 0.0493	0.169 ± 0.0584	0.729 ± 0.253	0.409 ± 0.163	0.275 ± 0.120	45.7 ± 16.8	48.1 ± 17.8
东方	nd	0.0392 ± 0.00942	nd	nd	nd	0.00386 ± 0.000329	nd	0.0412 ± 0.0152	nd	0.0225 ± 0.00461	0.0151 ± 0.00254	0.0405 ± 0.00520	0.0903 ± 0.00167	0.0105 ± 0.000243	0.00938 ± 0.000560	1.40 ± 0.123	1.66 ± 0.122
总检出率	85%	98%	86%	51%	60%	91%	45%	92%	88%	98%	99%	99%	100%	100%	95%	100%	100%

表2

图1

图2

表3

图3

图4

图5

图6

图7

图8

图9

图10

图11

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采样点		DBDPE	BTBPE	HBB	PBT	PBEB	∑ABFRs
福建	福鼎	3.15±0.612	0.0182±0.00118	nd	nd	nd	3.18±0.610
	泉州	3.83±0.543	0.0428±0.00907	0.0123±0.00144	nd	nd	3.88±0.550
	龙海	26.7±4.58	0.114±0.0336	nd	nd	nd	26.8±4.60
	漳江口	4.58±1.56	0.0438±0.0112	0.00838±0.00245	nd	nd	4.63±1.57
广东	深圳	29.4±1.71	1.11±0.366	0.205±0.0444	0.0243±0.00116	0.0257±0.00874	30.8±1.93
	广州	16.5±5.07	0.839±0.360	0.571±0.152	0.0242±0.00194	0.00409±0.000235	17.8±5.38
	珠海	8.71±2.23	0.0706±0.0145	0.0385±0.00710	nd	0.00427±0.000800	8.83±2.23
广西	山口	1.34±0.332	0.0144±0.00242	0.0284±0.0108	nd	nd	1.37±0.332
	北海	4.69±0.309	0.264±0.236	nd	nd	0.0163±0.0102	4.97±0.260
	钦州	1.82±0.363	0.0234±0.0103	nd	nd	0.00302±0.000476	1.84±0.370
	防城港	0.899±0.277	0.0217±0.00989	0.0113±0.00188	nd	nd	0.933±0.279
	北仑河口	0.516±0.0382	0.0255±0.00946	nd	nd	nd	0.532±0.0455
海南	花场	0.489±0.0198	0.0127±0.00449	0.00344±0.000448	nd	nd	0.501±0.0167
	文昌	1.61±0.860	0.164±0.137	nd	0.00978±0.00114	nd	1.79±0.882
	三亚	5.44±2.19	0.123±0.0595	nd	0.0303±0.0159	nd	5.59±2.25
	东方	0.552±0.0146	0.0198±0.00883	nd	0.0101±0.00104	nd	0.578±0.0214
总检出率		100%	92%	59%	33%	42%	100%

中国典型红树林沉积物中多溴联苯醚和替代型溴系阻燃剂污染特征

Pollution characteristics of polybrominated diphenyl ethers and alternative brominated flame retardants in sediments from typical mangrove wetlands of China

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