| 陈铭聪,杨东升,亦如瀚.排放管控前后电子垃圾回收区农业土壤中PBDEs时空分布变化动态[J].农业环境科学学报,2021,40(8):1718-1728. |
| 排放管控前后电子垃圾回收区农业土壤中PBDEs时空分布变化动态 |
| Temporal and spatial distribution dynamics of PBDEs in agricultural soil of e-waste recycling area before and after emission control |
| 投稿时间：2021-03-04 |
| DOI：10.11654/jaes.2021-0255 |
| 中文关键词: 多溴联苯醚 电子回收区 时空分布 逸度模型 一溴联苯醚 |
| 英文关键词: PBDEs e-waste recycling area spatial and temporal distribution multi-media fugacity model mono-BDE |
| 基金项目:国家自然科学基金项目（21637001） |
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| 中文摘要: |
| 为探明排放强度得到控制后，多溴联苯醚（Polybrominated diphenyl ethers，PBDEs）在典型电子垃圾回收区农业土壤中的时空分布变化特征及其迁移转化情况，根据2010年本课题组布置的采样点进行二次布点，于2017年8月在贵屿及周边区域采集了74份土壤样品，共测得55种PBDEs浓度数据。利用主成分分析、Pearson相关分析解析了55种PBDEs的潜在来源；通过与2010年所测数据对比，利用地理信息系统（GIS）研究区域土壤中PBDEs的时空分布变化特征；以BDE209为例，建立环境多介质逸度模型模拟其在介质间迁移转化的动态。结果表明：一到十溴联苯醚的几何平均浓度范围为0.08~42.27 ng·g-1，相比于2010年的0.03~230.00 ng·g-1，最大值明显降低；源解析结果显示，贵屿农业土壤可能仍受商用五、十溴联苯醚工业品影响，且该地区的PBDEs的降解过程可能为一个逐步、连续的脱溴反应；PBDEs时空分布特征显示，从2010年到2017年间，一溴联苯醚在研究区域土壤内浓度呈增加趋势，污染均匀扩散到全研究区，其他溴代的PBDEs浓度多以贵屿镇为中心显示岛状分布向周围扩散并呈下降趋势；多介质逸度模型模拟结果表明BDE209在研究区域中主要汇集于土壤和沉积物中，且其消失途径以土壤降解为主；通过一溴联苯醚储量估算，其在贵屿地区一年间（2020年）的新增储量保守估算仍有0.42 t。本研究表明，排放强度得到控制后，土壤中PBDEs的最主要组分BDE209及其他高溴代PBDEs会逐级脱溴降解为低溴代PBDEs，最终转化为一溴联苯醚（BDE1、BDE2、BDE3），已有研究证实其具有生物毒性，目前对人类的毒理学研究尚为空白，应该引起足够的关注。 |
| 英文摘要: |
| To investigate temporal and spatial distribution characteristics, the migration and transformation of polybrominated diphenyl ethers(PBDEs) in agricultural soils of typical e-waste dismantling areas after emission intensity was controlled. A total of 74 soil samples were collected in Guiyu and its surrounding areas in August 2017 based on the sampling sites arranged by the same research group in 2010. A total of 55 PBDE concentrations in the soil samples were determined, and Pearson correlation analysis and principal component analysis were used to identify potential sources of the 55 PBDEs. The spatial and temporal distribution characteristics of PBDEs in the soil of the research area were studied using a geographic information system(GIS) and compared with the 2010 data sets. In addition, an environmental multi-media fugacity model was used to simulate the migration and transformation dynamics of PBDEs among media, using decabrominated diphenyl ether(Deca-BDE, BDE209) as an example. Results showed that the geometric mean concentrations of Mono to Deca-BDE ranged from 0.08 to 42.27 ng·g-1, compared to the 2010 values(0.03 to 230 ng·g-1), where the maximum value decreased significantly. Source apportionment resulted in the cultivated soil in Guiyu being affected by commercial pentabrominated diphenyl ether and decabrominated diphenyl ether. The degradation process of PBDEs in this area might be a gradual and continuous debromination reaction. The spatial and temporal distribution characteristics of monobrominated diphenyl ether (mono-BDE) showed that the concentration in the soil within the study area increased from 2010 to 2017, and the pollution spread evenly throughout the study area. On the other hand, the concentration of the other PBDEs was mainly found in Guiyu Town, showing an island distribution that diffused to the surrounding area and exhibited a downward trend. The simulation results of the multi-media fugacity model showed that BDE209 mostly accumulated in soil and sediment;its disappearance pathway was mostly soil degradation. According to the estimation of Mono-BDE reserves, the newly increased reserves in Guiyu area in one year(2020) reached 0.42 t. The study results show that after the emission intensity was controlled, BDE209 and other highly brominated PBDEs in the soil debrominated and degraded into low-brominated PBDEs step by step, and finally converted to mono-BDE (BDE1, BDE2, and BDE3). Previous studies have confirmed that mono-BDE is biologically toxic. However, toxicological research on Mono-BDE in humans is still lacking, and more attention should be paid to it. |
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