济南市大气PM2.5铅污染特征、变化趋势与风险评估

Pollution characteristics, long-term variation trend, and health risk assessment of lead in ambient PM2.5 in Jinan

  • 摘要:
    背景 多项研究表明大气PM2.5中重金属对人群健康有影响,而PM2.5中铅污染长期低浓度暴露对人群健康影响的研究有限。
    目的 探讨济南市大气PM2.5中铅污染特征,评估其慢性健康风险。
    方法 收集济南市2014—2019年逐日PM2.5质量浓度(后称浓度)数据,分析PM2.5浓度的逐年变化趋势;另在济南市的主要工业区(历城区)和生活区(市中区)分别设置一个监测点,于2014—2019年的每个月10—16日采样(共采样493 d,部分缺失;其中采暖期172 d,非采暖期321 d)。每个监测点每天采集2个PM2.5样品,分别采用石英纤维滤膜用于铅的检测,玻璃纤维滤膜用于PM2.5浓度测定,共采集986份样品。采样仪器为100 L·min−1的大流量PM2.5采样器,每天累计采样时间为20~24 h。采用称重法测量PM2.5浓度,电感耦合等离子体质谱法测定PM2.5样品中铅浓度。分析2014—2019年PM2.5中铅的年平均浓度、富集因子水平与单位质量PM2.5中铅水平变化趋势以及采暖期与非采暖期的差异等。利用WS/T 777—2021《化学物质环境健康风险评估技术指南》评估大气PM2.5中铅的健康风险。
    结果 PM2.5中铅的年平均浓度范围为23.2~154.7 ng·m−3;2015—2019年采暖期平均浓度高于非采暖期,2015年、2017—2019年差异有统计学意义(P<0.01或0.001)。2014—2019年铅的富集因子范围为200~1342;在2015年、2017—2018年采暖期该因子高于非采暖期,差异有统计学意义(P<0.05或0.001)。单位质量PM2.5中铅水平为493~1944 ng·mg−1,2014年、2017—2018年采暖期和非采暖期其均值的差异均有统计学意义(P<0.05或0.001)。PM2.5中铅的年平均浓度和富集水平的年度变化呈下降趋势,单位质量PM2.5中铅水平也呈下降趋势。2014—2019年,济南市PM2.5中铅的致癌风险范围为1.69×10−8~2.45×10−6,整体趋势逐年下降,第95百分位数环比下降3%~46%。2017年以后,PM2.5中铅暴露的人群致癌风险降至可接受水平(<1×10−6)。
    结论 2015—2019年,采暖期PM2.5中铅浓度、富集因子大多较非采暖期升高,但单位质量PM2.5中铅水平变化不完全一致。2014—2016年,铅暴露对人群健康有致癌风险;2017年以后,PM2.5中铅暴露对人群的致癌风险处于可接受水平。

     

    Abstract:
    Background A number of studies have shown that heavy metals in atmospheric PM2.5 have impacts on human health, while studies on the impact of long-term and low-concentration exposure to lead in PM2.5 on human health are limited.
    Objective To investigate the pollution characteristics of lead in ambient PM2.5 and assess its chronic health risks.
    Methods Daily PM2.5 concentration data in Jinan from 2014 to 2019 were collected, and the year-by-year trend of PM2.5 concentration was analyzed. Licheng District (an industrial area) and Shizhong District (a residential area) were elected to install an ambient PM2.5 monitoring stationrespectively. The sampling instrument was a 100 L·min−1 high-flow PM2.5 sampler, with a cumulative sampling time of 20-24 h per day, using a quartz fiber filter membrane for lead detection and a glass fiber filter membrane for PM2.5 determination. The sampling frequency was 7 consecutive days per month from the 10th to the 16th (A total of 493 d were sampled and some were missing; 172 d during the heating period and 321 d during the non-heating period). Two PM2.5 samples were collected in one monitoring site each day. A total of 986 samples were collected in one monitoring site. The lead content in PM2.5 samples was detected by inductively coupled plasma mass spectrometry. The concentration of PM2.5 was measured by weighing method. The annual average concentration and enrichment factor of lead in PM2.5, the change trend of lead content per unit mass of PM2.5, and the difference between heating period and non-heating period from 2014 to 2019 were estimated. Technical guide for environment health risk assessment of chemical exposure (WS/T 777-2021) was used to assess the health risks of exposure to lead in PM2.5.
    Results The average annual concentration of lead in PM2.5 ranged from 23.2 ng·m−3 to 154.7 ng·m−3. The average concentration in heating period from 2015 to 2019 was higher than that in non-heating period, and the differences in 2015, 2017, and 2019 were statistically significant (P < 0.01 or 0.001). The enrichment factors ranged from 200 to 1342 in 2014 to 2019. The average enrichment factors in heating period in 2015, 2017, and 2018 was higher than those in non-heating period, and the difference was statistically significant (P < 0.05 or 0.001). The lead contents per unit mass of PM2.5 ranged from 493 ng·mg−1 to 1944 ng·mg−1, and the differences between heating period and non-heating period in 2014, 2017, and 2018 were statistically significant (P < 0.05 or 0.001). The average annual concentration and enrichment factor of lead in PM2.5 showed a downward trend, and thus the lead content per unit mass of PM2.5 also decreased. From 2014 to 2019, the carcinogenic risk of lead in PM2.5 in Jinan ranged from 1.69×10−8 to 2.45×10−6, showing a significant downward trend year by year, and the 95th percentile decreased by 3%-46% from the previous year. The carcinogenic risk level of lead was reduced to an acceptable level (<1×10−6) after 2017.
    Conclusion From 2015 to 2019, lead concentration and enrichment factor in PM2.5 increase during heating period compared with non-heating period, but it is not completely consistent of lead content in PM2.5 per unit mass. From 2014 to 2016, exposure to lead in PM2.5 may elevate carcinogenic risk to human. After 2017, the carcinogenic risks of exposure to lead in PM2.5 are at an acceptable level.

     

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