Pollution Characteristics and Risk Assessment of Flame Retardants in Middle and Upper Reaches of Beijiang River Basin
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摘要: 为探究北江中上游流域的阻燃剂污染状况和风险水平，采用气相色谱-串联质谱(GC-MS/MS)法测定了34个地表水样品和8个沉积物样品中31种阻燃剂的浓度，包括多溴联苯醚(PBDEs)、六溴环十二烷(HBCD)、四溴双酚A (TBBPA)这3种溴代阻燃剂和28种有机磷阻燃剂(OPFRs). 采用风险熵法评估了水体中阻燃剂的生态风险，并结合日饮用剂量评估了健康风险. 结果表明：①地表水中PBDEs和HBCD浓度范围分别为4.78~625.52、225.43~2 209.18 ng/L，未检出TBBPA；沉积物中PBDEs、HBCD和TBPPA含量范围分别为ND~11.82、121.13~395.86和ND~3.30 ng/g. ②地表水中OPFRs浓度范围为85.80~992.82 ng/L，浓度最高的3种单体分别为TCEP、TPhP和TDCIPP；沉积物中OPFRs含量范围为102.19~748.17 ng/g，含量最高的3种单体分别为TEHP、EHDPP和TCPP. ③对于地表水中已知毒性参数和健康数据的阻燃剂污染物，其生态风险总体处于中低水平，但BDE-100呈现出高风险，TTP呈现出中风险；其致癌风险和非致癌风险指数均处于可接受范围内，经饮水摄入造成的健康风险可以忽略. 研究显示，北江中上游流域阻燃剂污染程度较高，部分物质存在中高水平的生态风险，需要进一步关注.
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关键词:
- 北江 /
- 溴代阻燃剂(BFRs) /
- 有机磷阻燃剂(OPFRs) /
- 污染特征 /
- 风险评估
Abstract: In order to investigate the pollution status and risk level of flame retardants in the middle and upper reaches of the Beijiang River, gas chromatography-tandem mass spectrometry (GC-MS/MS) was used to determine the concentrations of 31 monomers of flame retardants, including three brominated flame retardants, i.e., polybrominated diphenyl ethers (PBDEs), hexabromocyclododecane (HBCD) and tetrabromobisphenol A (TBBPA), and 28 monomers of organophosphorus flame retardants (OPFRs). Ecological risks of flame retardants were assessed using risk entropy method and health risks were evaluated with daily drinking water. The results showed that: (1) PBDEs and HBCD concentrations in surface water ranged from 4.78-625.52 ng/L and 225.43-2209.18 ng/L, respectively, and no TBBPA was detected. The contents of PBDEs, HBCD and TBPPA in sediments ranged from ND-11.82 ng/g, 121.13-395.86 ng/g, and ND-3.30 ng/g, respectively. (2) The concentrations of OPFRs in surface water ranged from 85.80-992.82 ng/L, with TCEP, TPhP, and TDCIPP being the three most abundant monomers. The contents of OPFRs in sediment ranged from 102.19-748.17 ng/g, among which TEHP, EHDPP, and TCPP were the three most abundant monomers. (3) For flame retardants with available ecological and health risk data, the ecological risk of surface water was mainly at low and medium levels, BDE-100 was high risk, and TTP was medium level. The carcinogenic and non-carcinogenic risk indices were within acceptable range, and the health risk caused by drinking water was negligible. To sum up, flame retardant contamination in the middle and upper reaches of the Beijiang River is at a high level, and some substances have medium and high ecological risks, which deserve further attention. -
图 2 地表水和沉积物中不同种类阻燃剂占比
Figure 2. Percentage of flame retardants in surface water and sediments
图 3 北江地表水中阻燃剂空间分布
Figure 3. Spatial distribution of FRs in surface water of Beijiang River
图 5 地表水中阻燃剂非致癌风险分布
Figure 5. Distribution of Non-carcinogenic risk of flame retardants in surface water
图 6 地表水中阻燃剂致癌风险分布
Figure 6. Distribution of carcinogenic risk of flame retardants in surface water
表 1 检测的BFRs和OPFRs种类
Table 1. Types of BFRs and OPFRs detected
项目 种类 溴代阻燃剂(BFRs) 六溴环十二烷(HBCD) — 四溴双酚A(TBBPA) — 多溴联苯醚(PBDEs) BDE-28、BDE-47、BDE-99、BDE-100、BDE-153、BDE-154、BDE-183、BDE-209 有机磷阻燃剂(OPFRs) 烷基有机磷阻燃剂(Alkyl-OPFRs) 磷酸三甲酯(TMP)、磷酸三乙酯(TEP)、磷酸三正丙酯(TnPP)、磷酸三异丙酯(TiPP)、磷酸三正丁酯(TnBP)、磷酸三异丁酯(TiBP)、磷酸三戊酯(TPeP)、磷酸三己酯(THP)、磷酸三(2-乙基己基)酯(TEHP)、磷酸三(2-丁氧基乙基)酯(TBOEP)和磷酸二(2-乙基己基)酯(BEHP) 氯代有机磷阻燃剂(Chlorinated-OPFRs) 磷酸三(2-氯乙基)酯(TCEP)、磷酸三(2-氯异丙基)酯(TCPP)和磷酸三(1,3-二氯异丙基)酯(TDCIPP) 芳基有机磷阻燃剂(Aryl-OPFRs) 磷酸三苯酯(TPhP)、磷酸三邻甲苯酯(o-TTP)、磷酸三间甲苯酯(m-TTP)、磷酸三对甲苯酯(p-TTP)、2-乙基己基二苯基磷酸酯(EHDPP)、磷酸甲苯基二苯酯(CDPP)、磷酸异丙基二苯酯(IPDP)、磷酸叔丁基苯二苯酯(BPDP)、磷酸异癸基二苯酯(IDDP)、磷酸三(二甲苯)酯(TXP)、磷酸三(2-异丙基苯)酯(TIPPP)、磷酸三(3,5-二甲基苯基)酯(TDMPP)、磷酸二苄酯(DBPP)和三苯基氧化膦(TPPO) 
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表 2 4种目标化合物原始毒性数据
Table 2. Toxicity data of four target compounds
目标化合物 CAS 测试终点 浓度/
(mg/L)测试对象 BDE-28 41318-75-6 LC50 0.08217 大型溞(Daphnia magna) BDE-100 189084-64-8 LC50 0.01465 大型溞(Daphnia magna) TEHP 78-42-2 EC50 10 梨形四膜虫(Tetrahymena
pyriformis)EHDPP 1241-94-7 LC50 0.15 大型溞(Daphnia magna)
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表 3 阻燃剂的生态和健康风险评估参数
Table 3. Data for ecological and health risk assessment of flame retardants
目标化合物 PNEC/(ng/L) SFO/(kg·d/ng) RfD/[ng/(kg·d)] BDE-28 82.17[29-30] na na BDE-100 14.65[29-30] na na HBCD na na 22 000[24] TEHP 10 000[29-30] 3.10×10−9[27] 100 000[27] TDCIPP 12 400[25] 3.10×10−8[27] 20 000[27] o-TTP 32[25] na 13 000[28] m-TTP 32[25] na 13 000[28] p-TTP 32[25] na 13 000[28] TCEP 5 000[25] 2.00×10–8[27] 7 000[27] TiBP 11 000[26] na na EHDPP 150[29-30] na 15 000[28] TEP 1 600 000[25] na 15 000[28] TCPP 120 000[25] na 10 000[27] TBEP 13 000[25] na 15 000[28] TnBP 66 000[25] 9.00×10−9[27] 10 000[27] TPhP 160[25] na 70 000[28] 注：na表示未查阅到相关数据.
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表 4 水和沉积物中BFRs暴露水平
Table 4. Exposure level of BFRs in surface water and sediments
BFRs种类 地表水 沉积物 浓度范围/(ng/L) 平均值/(ng/L) 检出率/% 含量范围/(ng/g) 平均值/(ng/g) 检出率/% PBDEs BDE-28 1.68~11.22 5.95 73.53 0.20~0.58 0.39 25.00 BDE-47 ND ND 0.00 ND ND 0.00 BDE-99 ND ND 0.00 ND ND 0.00 BDE-100 ND~625.52 145.77 96.97 1.40~11.82 5.00 87.50 BDE-153 ND ND 0.00 ND ND 0.00 BDE-154 ND ND 0.00 ND ND 0.00 BDE-283 ND ND 0.00 ND ND 0.00 BDE-209 ND ND 0.00 ND ND 0.00 ∑PBDEs 4.78~625.52 149.03 100.00 ND~11.82 4.47 87.50 HBCD 225.43~2 209.18 950.41 100.00 121.13~395.86 266.23 100.00 TBBPA ND ND 0.00 ND~3.30 2.97 25.00 注：ND表示该种污染物浓度低于检出限.
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表 5 水和沉积物中OPFRs的暴露水平
Table 5. Exposure levels of OPFRs in surface water and sediments
OPFRs 地表水 沉积物 浓度范围/(ng/L) 平均值/(ng/L) 检出率/% 含量范围/(ng/g) 平均值/(ng/g) 检出率/% TMP ND ND 0.00 ND ND 0.00 TEP 0.32 ~ 42.34 5.26 100.00 1.98 ~ 6.17 4.29 100.00 TnPP ND ~ 336.94 16.49 94.12 0.10 ~ 0.86 0.45 100.00 TiPP ND ~ 139.53 9.21 97.06 0.18 ~ 0.97 0.46 100.00 TnBP 1.42 ~ 173.14 36.03 100.00 11.79 ~ 19.01 16.57 100.00 TiBP 1.23 ~ 156.43 30.16 100.00 10.13 ~ 17.86 14.43 100.00 TPeP ND ~ 6.36 1.93 38.24 0.09 ~ 1.45 0.38 100.00 THP 0.16 ~ 31.48 6.44 100.00 ND ~ 0.22 0.09 62.50 TEHP 1.62 ~ 48.16 10.73 100.00 14.11 ~ 380.26 143.34 100.00 TBOEP 0.06 ~ 172.31 9.26 100.00 ND ND 0.00 TCEP ND ~ 356.10 61.88 85.29 3.17 ~ 20.73 11.00 100.00 TCPP 3.98 ~ 89.77 26.62 100.00 35.92 ~ 64.67 48.25 100.00 TDCIPP 3.16 ~ 241.06 42.32 100.00 ND ~ 54.14 7.23 25.00 TPhP 4.03 ~ 246.71 46.73 100.00 3.92 ~ 82.01 14.61 100.00 o-TTP ND ~ 10.51 5.54 8.82 ND ~ 1.17 0.15 12.50 m-TTP ND ~ 124.65 22.77 82.35 ND ~ 2.07 0.79 62.50 p-TTP ND ~ 146.49 24.89 85.29 0.52 ~ 6.56 2.99 100.00 EHDPP 0.23 ~ 7.12 1.41 100.00 0.90 ~ 228.22 57.78 100.00 CDPP ND ND 0.00 ND ~ 51.36 6.42 12.50 IPDP ND ~ 65.29 23.58 41.18 ND ND 0.00 BPDP ND ~ 97.31 53.74 23.53 ND ~ 47.79 5.97 12.50 IDDP ND ~ 2.36 0.67 26.47 ND ~ 3.83 0.48 12.50 TXP ND ~ 26.25 7.72 44.12 ND ~ 3.43 1.52 25.00 TIPPP ND ~ 167.24 43.79 55.88 ND ND 0.00 TDMPP ND ~ 28.41 9.13 38.24 ND ~ 1.78 0.22 12.50 DBPP ND ~ 86.70 39.70 20.59 ND ND 0.00 TPPO 2.83 ~ 102.63 30.75 100.00 ND ~ 3.04 1.53 12.50 BEHP 0.03 ~ 0.98 0.22 100.00 0.74 ~ 19.96 7.54 100.00 ∑OPFRs 85.80 ~ 992.82 426.47 100.00 102.19 ~ 748.17 346.46 100.00 注：ND表示该种污染物浓度低于检出限，未检出.
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