Exposure of Mother and Infants to Polycyclic Aromatic Hydrocarbons during Lactation, Beijing
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摘要: 多环芳烃（PAHs）是一类普遍存在于水圈、生物圈、岩石圈和大气圈的持久性有机污染物，并在各种环境介质中交换、迁移，从而影响人体健康。以母乳为介质，评价哺乳期女性和婴幼儿PAHs暴露风险具有重要意义。早期研究表明，北京母乳中PAHs浓度在全球范围内处于较高水平。本文项目组在2012-2016年间，连续采集北京地区30位哺乳期女性6个月母乳，并检测其中PAHs浓度，旨在掌握该地区母乳中PAHs残留水平、婴幼儿的暴露量，以及哺乳期母体和婴幼儿暴露风险的变化趋势与特征。通过对30位女性分娩后连续6个月内180个母乳中15种PAHs的监测，采用气相色谱-质谱法（GC-MS）测定其含量，初步研究结果表明：①15种PAHs都有检出，其中检出浓度和检出率高的单体化合物包括菲、芴、苊烯、蒽、苊和荧蒽。母乳样品中Σ15PAHs的浓度均值为348μg/kg脂质，与2005年该地区的报道值相比有下降趋势。②15种PAHs和7种高致癌活性PAHs的苯并[a]芘的等效致癌活性（BaPeq）浓度分别为8.53μg/kg脂质和7.89μg/kg脂质，婴幼儿每日暴露估算值分别为1.51μg/day/kg b.w.和0.19μg/day/kg b.w.，均比2005年有所下降，但高于捷克、美国、土耳其等国家婴幼儿在母乳喂养期的暴露量，低于我国兰州等重工业城市最新暴露量研究结果。③整个哺乳期，母乳中PAHs的总浓度没有明显下降趋势，但冬季可能由于采暖增加了大气中PAHs的排放，使得母乳样品中15种PAHs总浓度明显高于夏季、秋季和春季。SPSS双变量相关分析结果表明，母乳中15种PAHs的总浓度与母体年龄、身体质量指数和母乳脂肪含量不存在相关性。未来工作中需要更加充足的样品分析数据进一步证实以上研究结果。要点
(1) 北京哺乳期女性及婴幼儿PAHs暴露量和暴露风险与早期相比呈下降趋势。
HIGHLIGHTS(1) For mother and breast-feeding infants, the exposure dose and risk to PAHs were decreasing.
Abstract:BACKGROUNDPolycyclic aromatic hydrocarbons (PAHs) are classic persistent organic pollutants in the hydrosphere, lithosphere, biosphere and atmosphere, which have a harmful effect on human health by exchanging and migrating among various environmental media. Breast milk is an ideal biometric to monitor the exposure risk of mothers and infants to PAHs. Earlier research indicated that the residue levels of PAHs in breast milk from Beijing were higher in the world.OBJECTIVESTo understand the changes in the residue levels of PAHs in breast milk in the region, the exposure of infants, and the trends and characteristics of the exposure risk of breastfeeding mothers and infants.METHODSFor 30 first-delivery women in Beijing, a breast milk sample per month within 180 days postpartum period was collected. The PAHs and fat content of breast milk were determined by gas chromatography-mass spectrometry (GC-MS) and monitored to study the time tendency of PAHs and estimate the exposure risk of infants to PAHs.RESULTSThe dominant pollutants were acenaphthylene, acenaphthene, fluorene, phenanthrene, anthracene, and fluoranthene. The average concentration of Σ15PAHs in 180 samples was 348μg/kg lipid, which was lower than the value reported in 2005. Compared to the early reported residue level, the BaP-equivalent (BaPeq) concentrations decreased, which were 7.89μg/kg lipid for seven carcinogenic compounds, and 8.53μg/kg lipid for 15 PAHs. For breastfeeding infants in Beijing, the mean acceptable daily intakes (EDIs) of Σ15PAHs and Σ7PAHs through breast milk were 1.51μg/day/kg b.w. and 0.19μg/day/kg b.w., respectively, which was lower than those in 2005. However, it was higher than the exposure of infants in some countries such as Czech, America, Turkey during breastfeeding, and lower than the latest research results of Lanzhou and other heavy industrial cities in China. Throughout the lactation period, the total concentration of PAHs in breast milk did not decrease significantly, but winter heating may increase the emission of PAHs in the atmosphere, making the total concentration of 15 PAHs in breast milk samples significantly higher than that in summer, autumn, and spring.CONCLUSIONSBivariate correlations analytical results show that the concentration of Σ15PAHs is not associated with age, BMI and lipid content. Limited by sample size, those results should be confirmed with perfect experiment design and sufficient samples in future studies.
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江西西北部是我国重要的铌钽铍锂稀有金属成矿区之一，该地区锂及稀有金属矿成矿地质条件优越，区内产有闻名全国的宜春414、同安等超大型稀有金属矿床及众多含锂瓷石矿床[1]，且矿床类型较多。赣西北地区的稀有金属成矿作用主要集中于两个地区[2-4]：①武功山成矿带，414特大型稀有金属矿床就产于其中，该成矿带的稀有金属成矿作用与雅山花岗岩有关，岩体位于武功山复背斜的北东端南东翼；②九岭成矿带，稀有金属矿化发生在燕山期花岗岩浆活动晚阶段形成的碱长花岗岩及更晚期的细晶花岗岩脉中，这类矿化岩体进一步可分为铁锂云母-(锂)白云母碱长花岗岩、锂云母碱长花岗岩和花岗细晶岩脉等。自2012年以来，中国地质调查局设立三稀项目，继续把这一带作为重点工作区，开展综合研究和重点评价，期望取得找矿新进展。
华南重点矿集区稀有稀散和稀土矿产调查项目组对位于江西九岭山东南侧的宜丰、上高等地的二云母碱长花岗岩、锂(白)云母碱长花岗岩、黄玉锂云母碱长花岗岩开展了野外调查，并结合实验室综合研究尤其是镜下鉴定、电子探针和化学分析，发现了磷锂铝石、锂云母、绿柱石、富钽锡石、铌钽铁矿-钽铌铁矿系列矿物，初步证明了可利用工业矿物的存在。
磷锂铝石是一种含锂和铝的磷酸盐矿物，标准化学式为LiAl[PO4](F)，其中Li可被Na置换，F可被(OH)置换而逐渐变为羟磷锂铝石[5]。磷锂铝石在稀有金属花岗伟晶岩中较常见[6]，晶体粗大，有的以米来度量。这种矿物的特点之一是Li2O含量很高，一般可达10%，高于常见的锂矿物锂辉石(Li2O含量7%)，因而是一种重要的工业锂矿物。本次工作在九岭成矿带首次发现的磷锂铝石，在二云母碱长花岗岩、锂(白)云母碱长花岗岩、黄玉-锂云母碱长花岗岩中均有出现，其在黄玉-锂云母碱长花岗岩中的含量更是高达4%~5%，可列为造岩矿物。镜下观察磷锂铝石多为半自形板柱状，晶体一般在0.2~0.8 mm，有时可见极细密的聚片双晶，正突起低至中度，正交偏光下干涉色均在一级顶部。电子探针和LA-ICP-MS分析表明其主要成分Al2O3含量变化于35.90%~39.09%，平均值37.59%；P2O5含量变化于45.34%~50.95%，平均值48.81%；Li2O含量变化于7.41%~11.55%，平均值9.58%。
锂(白)云母在九岭成矿带也是广泛分布的一种矿物，镜下观察呈片状，形成晚于长石，数量在9%左右，最高可达15%。LA-ICP-MS分析表明锂(白)云母中的Li2O含量约4.5%，因其在岩石中的含量较高，因而也是九岭地区重要的锂工业矿物。
绿柱石又称“绿宝石”，是铍-铝硅酸盐矿物，在九岭成矿带稀有金属花岗岩中属首次发现，主要见于二云母碱长花岗岩和黄玉锂云母碱长花岗岩中。在薄片中矿物的切面恰好垂直于C轴方向而呈均质体，属岩浆结晶产物。本次九岭地区绿柱石的发现表明本地区铍矿可能也具有一定找矿潜力。
锡石在九岭地区也普遍存在，主要见于黄玉-锂云母碱长花岗岩中。晶体较铌钽矿物粗大，分布于长石、云母粒间，有时也与黄玉关系密切。本地区含锂花岗岩中的锡石的Fe、Mn、Mg和Ti含量均不高，但Nb、Ta含量较高，尤其是Ta含量高达8.68%。锡石的发现不但为进一步寻找钽矿提供了线索，也为九岭山乃至区域上寻找锡矿提供了依据。
铌钽矿物主要见于黄玉-锂云母碱长花岗岩中，含量不高，但普遍存在；据电子探针分析，属于铌钽氧化物中的铌钽铁矿族，既有富钽矿物，也有富铌矿物，总体上Ta和Mn呈正相关，所以富钽矿物均为铌钽锰矿。富铌矿物既有钽铌锰矿，也有钽铌铁矿，属于岩浆晚期富挥发组分结晶分异的成因。
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图 1 江西九岭山上高—宜丰一带稀有金属矿物的镜下特征Figure 1. Arthroscopic characteristics of the rare metal minerals in the Jiuling area, Jiangxi Province赣西北地区的稀有金属成矿作用主要集中于武功山成矿带和九岭成矿带，以往的工作多集中在武功山成矿带，相对来说九岭成矿带的研究程度较低，尤其是矿物学的认识少。本次工作对九岭成矿带与稀有金属成矿关系密切且广泛分布的二云母碱长花岗岩、锂(白)云母碱长花岗岩、黄玉锂云母碱长花岗岩开展研究，发现了重要含锂矿物——磷锂铝石的大量存在，以及绿柱石、富钽锡石、铌钽铁矿、钽铌铁矿等工业稀有金属矿物及相关金属矿物的普遍存在，为该地区Li、Be、Ta及Sn的找矿工作部署提供了直接依据。另外，研究表明黄玉、萤石等富含B、P络合剂元素的矿物在九岭成矿带也常见，可作为找矿标志矿物。
近两年来国内外对硬岩型锂矿的研究与勘查高度关注[7-9]，而磷锂铝石型锂矿类型的查证及开发利用将有助于改变锂矿资源的格局，为新兴产业的发展提供新的资源保障。
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图 1 不同月份(a)与季节(b)母乳中PAHs的浓度均值和相对偏差
Figure 1. Average concentration of total PAHs in breast milk collected in (a) different month and (b) season. Error bars represent the standard deviation (SD)
表 1 志愿者和母乳采样信息
Table 1 Main information of breast milk in the donors
参数 范围 志愿者数量(名) 30 样品量(个) 180 样品采集时间(年) 2012—2016 年龄(岁) 26~36 (30±2.3)a BMI(kg/m2) 22.0~28.5 (26.1±2.9)a 身高(cm) 152~172 (161±4.7)a 春季样品量(3月~5月，个) 44 夏季样品量(6月~8月，个) 36 秋季样品量(9月~10月，个) 35 冬季样品量(11月~次年2月，个) 65 注：a为年龄等的均值，BMI为身体体重指数(体重/身高2, kg/m2)。 
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表 2 样品中PAHs浓度分析结果
Table 2 Concentrations of target compounds in 180 human breast milk samples
PAHs化合物 均值(μg/kg脂质) 中位值(μg/kg脂质) 最小值(μg/kg脂质) 最大值(μg/kg脂质) 检出率(%) 占比(%) 苊 26.4 18.8 NDa 110 68.9 7.59 苊烯 49.9 47.2 ND 180 77.2 14.3 芴 63.0 62.0 ND 151 96.7 18.1 菲 91.2 90.4 8.66 245 100 26.2 蒽 35.3 26.8 2.15 110 100 10.1 荧蒽 21.3 15.5 ND 90.7 93.9 6.11 芘 16.4 12.3 ND 113 77.2 4.71 苯并[a]蒽 7.56 6.02 ND 50.7 58.3 2.17 䓛 11.7 8.86 ND 64.0 66.7 3.37 苯并[b]荧蒽 9.26 5.17 ND 88.4 60.6 2.66 苯并[k]荧蒽 8.46 3.21 ND 79.8 49.4 2.43 苯并[a]芘 1.98 ND ND 17.7 25.0 0.57 茚苯(1, 2, 3-cd)芘 1.95 ND ND 14.6 30.6 0.56 二苯并[a, h]蒽 2.69 ND ND 13.6 38.9 0.77 苯并[ghi]苝 1.20 ND ND 10.5 23.3 0.34 Σ PAHs 348 296 70.3 745 - - 注：ND表示未检出。
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表 3 不同地区母乳样品中15种PAHs和7种PAHs的BaPeq值
Table 3 BaPeq values of 15 PAHs and 7 PAHs in human milk from different areas
采样地区 BaPeq(μg/kg脂质) 7种PAHs的占比(%) 样品量(个) 参考文献 15种PAHs 7种PAHs 北京 8.53 7.89 92.5 180c 本文 北京 9.08a 8.60a 94.6 40 [35] 日本 1.45b 1.44b 99.3 51 [34] 西班牙(初乳) 7.53b 7.07b 93.9 18 [33] 香港 13.6 12.1 89.8 29 [38] 捷克 0.41a 0.38a 92.7 188 [32] 兰州 54.2a 53.7a 99.1 98 [39] 土耳其 0.59 0.54 91.5 47 [10] 意大利 201a, b 187a, b 93.0 30 [31] 美国 0.02 0 0 12 [37] 注：a为根据文献中报道的均值计算所得；b为根据文献中单位体积PAHs浓度，以3.6%的脂肪含量计算；c为本文180个样品的测定均值。
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