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十溴二苯乙烷(decabromodiphenyl ethane,DBDPE)属于新型溴系阻燃剂(new brominated flame retardants,NBFRs)的一种,于1990年初开始作为十溴联苯醚(decabromodiphenyl ether, BDE-209)的替代品在商业上得到广泛应用[1]。DBDPE具有热稳定性好、抗紫外线能力强、渗出率低等优点,在高聚物合成材料、塑料、纤维、树脂、橡胶、建材等材料中都有所应用[2-3]。作为添加型阻燃剂,DBDPE以物理分散状态与基材共混,两者间没有化学键相连[4]。因此,在生产、使用和废物处置等环节,DBDPE都容易从产品中释放进入环境[5]。
近年来,随着BDE-209的逐步淘汰,DBDPE的生产和使用量逐年上升,其在大气、粉尘、土壤、沉积物、水体等环境介质中的检出浓度亦呈不断攀升的趋势。中国是溴系阻燃剂生产和使用大国,2006年至2016年DBDPE生产总量约23万吨,污染形势较国外更为严峻[6]。中国部分城市粉尘中DBDPE检出浓度已超过所有多溴联苯醚(poly brominated diphenyl ethers, PBDEs)的总和[7],杭州郊区土壤中DBDPE是检出浓度最高的新型溴系阻燃剂[8]。现有研究表明,DBDPE在生物体内也已广泛存在。如广东某电子垃圾回收站周边池塘鲤鱼肌肉组织中DBDPE的检出浓度为440—1000 ng·g−1(脂重)[9],青蛙体内的检出浓度为15.1—149 ng·g−1(脂重)[10]。浙江温岭电子拆解工人头发和血清中DBDPE的平均检出浓度分别为82.5 ng·g−1(干重)和125.2 ng·g−1(脂重)[11]。北京母乳样本中DBDPE检出率达100%,浓度为0.422—28.6 ng·g−1(脂重)[12]。
DBDPE具有持久性、生物积累性、毒性以及长距离迁移能力[4],因而对人类健康和生态环境存在潜在危害,由DBDPE引起的环境污染问题已经引起人们的高度重视。本文从污染现状、环境行为及风险评估3个方面对近年来有关DBDPE的研究进行了综述,为DBDPE的环境监管、DBDPE在环境和生物介质中的迁移转化和定向积累等行为与归趋研究提供相关资料,对科学评价DBDPE生态环境安全性具有重要意义。
十溴二苯乙烷的污染现状及环境行为研究进展
Research progress on the pollution status and environmental behaviors of decabromodiphenyl ethane
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摘要: 新型溴系阻燃剂十溴二苯乙烷(decabromodiphenyl ethane, DBDPE)是十溴联苯醚(decabromodiphenyl ether, BDE-209)的主要替代品,使用量和产量逐年上升,其环境安全性问题备受重视。本文在论述DBDPE基本理化性质及环境污染现状的基础上,系统总结了目前有关DBDPE在不同环境介质中的行为与归趋研究进展(如环境迁移、代谢与降解、动植物吸收富集等),并从风险熵法和危害指数法两个方面对有关DBDPE风险评估的研究进行了综述。最后,指出了当前研究存在的不足并对今后的研究方向作出展望。本文将有助于系统认识DBDPE的环境效应,为后续DBDPE环境行为研究及环境污染监管提供参考依据。Abstract: Decabromodiphenyl ethane (DBDPE), a novel brominated flame retardant, is a primary substitute for decabromodiphenyl ether (BDE-209). The use and production of DBDPE are increasing year by year, and its environmental safety has received extensive attention. This paper summarized the physicochemical properties and pollution status of DBDPE in the environment and reviewed the main research progress on the behaviors and fate of DBDPE in the environment (such as environmental transportation, metabolism, degradation, absorption, and bioaccumulation in plants and animals). It also summarized the research progress on DBDPE risk assessment basing on the risk quotient method and hazard index method. The existing problems and future research prospects were also discussed. The review will help better understand the environmental impacts of DBDPE and guide the subsequent study on its environmental behaviors and pollution supervision.
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表 1 DBDPE的物理化学性质
Table 1. Physicochemical properties of DBDPE
表 2 DBDPE在不同环境介质中的浓度
Table 2. Concentration of DBDPE in different environmental media
环境介质
Environmental media采样点
Sampling site中位数和/或浓度范围
Median and/or concentration range采样时间
Sampling time参考文献
Reference大气 爱尔兰垃圾填埋场 <0.9—2 pg·m−3 2018.11—2019.1 [22] 瑞典斯德哥尔摩(室外) 0.15 (<0.12—0.33) pg·m−3 2012 [23] 瑞典斯德哥尔摩(室内) <90—250 pg·m−3 2012 [23] 印度比哈尔邦(室内) 273 (116—15358) pg·m−3 2015.8—2015.10 [26] 中国广东广州工业园区 414 (57.6—2472) pg·m−3 2015—2016 [25] 巴基斯坦卡拉奇
电子垃圾回收站67.5 (8.5—99.5) ng·m−3 2014.8 [28] 中国山东DBDPE生产厂 213 (12.7—435) μg·m−3 2016 [27] 粉尘 英国伯明翰家庭 41 (<1.2—2300) ng·g−1 2015.2—2015.5 [33] 英国伯明翰办公室 440 (<1.2—17000) ng·g−1 2015.2—2015.5 [33] 澳大利亚墨尔本家庭 1600 (ND—9000) ng·g−1 2016.9 [60] 澳大利亚墨尔本办公室 1900 (ND—10000) ng·g−1 2016.9 [60] 澳大利亚墨尔本汽车 1900 (ND—3900) ng·g−1 2016.9 [60] 中国广州家庭 4600 (153—96410) ng·g−1 2015.9—2016.7 [61] 中国广东广州城市(室内) 727 (241—4420) ng·g−1 2013.9—2014.3 [31] 中国广东清远农村(室内) 665 (211—1900) ng·g−1 2013.9—2014.3 [31] 中国广东清远电子垃圾
回收站车间2720 (669—15000) ng·g−1 2013.9—2014.3 [31] 中国浙江、广东电子垃圾拆解场地 140—170000 ng·g−1 2013.7—2013.12 [32] 巴西垃圾填埋场 2664 (ND—5910) ng·g−1 2015 [62] 土壤 中国山东寿光DBDPE生产厂周边 610 (12—9000) ng·g−1(干重) 2014.8 [41] 澳大利亚墨尔本电子垃圾回收站周边 <45 (ND—37000) ng·g−1(干重) 2017.11 [34] 中国广东贵屿电子垃圾回收站周边(非根际土壤) 15.35 (7.33—134) ng·g−1(干重) 2012.12 [63] 土壤 中国广东贵屿电子垃圾回收站周边(根际土壤) 33.1 (10.1—348) ng·g−1(干重) 2012.12 [63] 巴西垃圾填埋场 1.7 (ND—83) ng·g−1(干重) 2015 [62] 中国山东寿光农田 12—344 ng·g−1(干重) 2008.5 [43] 中国青藏高原 <LOQ—1450 pg·g−1(干重) 2012.5 [44] 沉积物 中国广东广州红树林湿地 14.9 (3.7—26) ng·g−1(干重) 2015.11 [54] 中国广东珠海红树林湿地 9.33 (5.16—21.5) ng·g−1(干重) 2015.11 [54] 中国广东深圳红树林湿地 10.5 (7.7—14.41) ng·g−1(干重) 2015.11 [54] 南非瓦尔河 176.06 (59—350) ng·g−1(干重) 2017.10—2017.12 [50] 中国珠江三角洲地区 1.520—1714 ng·g−1(干重) 2013 [52] 中国大鹏湾 122.1 (4.37—276.4) ng·g−1(干重) 2013 [52] 中国黄海海湾 0.16—39.7 ng·g−1(干重) 2014 [53] 欧洲水产养殖场底泥 <0.01—2.41 ng·g−1(干重) 2016 [64] 水体 中国广东东江(颗粒相) 48 (37—110) ng·g−1 2010.5 [47] 中国广东东江(溶解相) 13 (13—38) pg·L−1 2010.5 [47] 中国渤海海水(溶解相) ND—91.44 pg·L−1 2016—2017 [48] 爱尔兰垃圾填埋场地下水 9.35 (1.3—630) ng·L−1 2018.11—2019.1 [22] 污水污泥 中国哈尔滨污水处理厂污水(入口) <LOQ—86.13 ng·L−1 2012—2013 [55] 中国哈尔滨污水处理厂污水(出口) <LOQ—17 ng·L−1 2012—2013 [55] 中国哈尔滨污水处理厂(好氧污泥) 50.8—911 ng·g−1(干重) 2012—2013 [55] 中国哈尔滨污水处理厂(脱水污泥) 57.6—577 ng·g−1(干重) 2012—2013 [55] 西班牙加泰罗尼亚污水处理厂污泥 62.5 (ND—257) ng·g−1(干重) 2009 [58] 中国广州污水处理厂污泥 4090 (675.4—27438.6) ng·g−1(干重) 2013—2014 [59] 韩国生活污水处理厂污泥 <LOQ—89.2 ng·g−1(干重) 2011.7—2011.10 [57] 韩国生活-工业混合污水处理厂污泥 <LOQ—108 ng·g−1(干重) 2011.7—2011.10 [57] 韩国工业污水处理厂污泥 <LOQ—3100 ng·g−1(干重) 2011.7—2011.10 [57] 澳大利亚污水处理厂生物固体 600 (ND—1100) ng·g−1(干重) 2017.9—2018.4 [60] 注:ND—未检出;LOQ—定量限.Note: ND—not detectable; LOQ—limit of quantitation. 表 3 不同文献中的DBDPE每日估计摄入量(EDI)
Table 3. Estimated daily intake (EDI) of DBDPE in different references
暴露途径
Exposure route样品信息
Sample information暴露人群
Exposed populationEDI/
(ng·kg−1·d−1·bw)参考文献
Reference灰尘摄入 广东,某高校17个大学宿舍室内灰尘 成人 0.58a, 1.46b [110] 广东,城市室内灰尘(n=28) 儿童 3.73a, 29.4b [31] 广东,城市室内灰尘(n=28) 成人 0.33a, 1.62b [31] 广东,电子垃圾回收站车间灰尘(n=20) 儿童 15.5a, 169b [31] 广东,电子垃圾回收站车间灰尘(n=20) 成人 1.35a, 9.27b [31] 广东,农村室内灰尘(n=30) 儿童 2.71a, 22.9b [31] 广东,农村室内灰尘(n=30) 成人 0.24a, 1.26b [31] 比利时、意大利和西班牙的室内灰尘(n=65) 儿童 0.404a, 3.19b [40] 比利时、意大利和西班牙的室内灰尘(n=65) 成人 0.0207a, 0.246b [40] 上海,室内地面灰尘(n=22) 从婴儿至成人 0.13—1.04a [39] 上海,室内桌椅等家具上灰尘(n=22) 从婴儿至成人 0.05—0.40a [39] 土壤摄入 华北,DBDPE生产厂周边土壤 成人 1.15b [42] 华北,DBDPE生产厂周边土壤 儿童 26.9b [42] 呼吸吸入 印度,城市建筑室内空气 儿童 0.534a, 8.546b [26] 印度,郊区建筑室内空气 儿童 0.199a, 0.638b [26] 印度,城市建筑室内空气 成人 0.140a, 2.234b [26] 印度,郊区建筑室内空气 成人 0.0519a, 0.167b [26] 山东,20个DBDPE生产厂车间空气 成人 11500a, 27500b [27] 华北,DBDPE生产厂周围空气 儿童 0.82b [111] 华北,DBDPE生产厂周围空气 成人 0.2b [111] 皮肤接触吸收 比利时、意大利和西班牙的室内灰尘(n=65) 儿童 4.14×10−4a, 1.64×10−3b [40] 比利时、意大利和西班牙的室内灰尘(n=65) 成人 2.39×10−5a, 9.44×10−5b [40] 北京,30个成人的手掌、手背及前臂表面擦拭样品 成人 7.0 ng·d−1a, 80.4 ng·d−1b [112] 饮食摄入 北京,20位母亲3 d重复饮食样品 母亲 23.5a, 506b [12] 北京,母乳(n=20) 婴儿(母乳喂养) 33.6a, 114b [12] 浙江,某农场温室蔬菜(番茄、黄瓜) NA 586—807 ng·d−1a [8] 浙江,某农场非温室蔬菜(番茄、黄瓜) NA 51—185 ng·d−1a [8] 注:NA—无资料;a.平均暴露量;b.日最高暴露量. Note: NA—not available; a. daily average intake; b. daily high intake. -
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