“三年行动计划”对大气环境持久性自由基污染特征和来源的影响

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摘要采用电子顺磁共振波谱法（EPR）对“打赢蓝天保卫战三年行动计划”（“三年行动计划”）实施期间（2018~2020年）以及实施前后（2017年和2021年）西安大气PM_2.5中EPFRs的浓度特征、种类特征及可能来源进行了探讨.结果发现，该计划实施后西安大气PM_2.5中EPFRs平均浓度（5.03×10¹⁴spins/m³）比实施前（7.18×10¹⁴spins/m³）下降了29.9%，表明“三年行动计划”的实施对EPFRs的控制是有效的.冬季浓度（8.61×10¹⁴spins/m³）是夏季（3.10×10¹⁴spins/m³）的2.8倍，其主要类型为以碳为中心附近受含氧官能团影响的自由基.相关性及平行因子分析显示，燃煤源（35.3%）、交通燃烧源（30.0%）和扬尘源（27.8%）可能是西安大气PM_2.5中EPFEs的主要来源.冬季交通燃烧源占比最高（45.8%），而夏季EPFRs与O₃相关性比较显著，二次来源占比在夏季是其他季节的2.2~5.7倍.该计划实施前后燃煤源占比明显下降（下降13.7%），说明清洁取暖、煤炭消费总量控制和燃煤锅炉综合整治等政策是非常有效的，但交通燃烧源（上升3.70%）、扬尘（上升3.00%）及二次来源（上升7.00%）略有上升，表明加强扬尘综合治理、控制机动车排放绿色出行以及控制O₃、VOCs等的污染是未来控制的重点.重污染天气下EPFRs的来源中燃煤源（42.9%）和扬尘源（33.4%）占比较高，而交通燃烧源（31.7%）和二次来源（8.95%）在优良天气的占比相对较高，说明不仅要减少重污染天气，优良天气中EPFRs对健康的影响也需要进一步关注.

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关键词 ：环境持久性自由基(EPFRs), PM_2.5, 污染特征, 来源, "三年行动计划"

Abstract：The concentration characteristics, species type, and potential sources of environmentally persistent free radicals (EPFRs) in atmospheric PM_2.5 of Xi'an were investigated during, before, and after the implementation of the Three-year Action Plan for Winning the Blue Sky Battle, using Electron paramagnetic resonance spectroscopy (EPR). Results showed that the mean concentration of EPFRs after the implementation of the plan (5.03×10¹⁴spins/m³) decreased 29.9% compared with that before the implementation (7.18×10¹⁴spins/m³), which suggests that EPFRs were effectively controlled due to the implementation of the Three-year Action Plan. The mean concentration of EPFRs in winter (8.61×10¹⁴spins/m³) was 2.8times that in summer (3.10×10¹⁴spins/m³), and the main type was the free radicals affected by oxygen-containing functional groups near the carbon atoms. Correlations and parallel factor analysis revealed that coal combustion (35.3%), traffic emission (30.0%), and dust (27.8%) were the main sources of EPFEs in atmospheric PM_2.5 of Xi'an. Traffic emission was the most dominant source of EPFRs in winter season (45.8%), whereas the EPFRs was strongly correlated with O₃ in summer season and the contribution of secondary sources was 2.2~5.7times that of other seasons. The contribution of coal combustion to EPFRs decreased significantly (13.7%) after the implementation of the plan, indicating that policies such as clean heating, total coal consumption control, and comprehensive improvement of coal-fired boilers were very effective. The contributions of traffic emission, dust, and secondary sources slightly increased (3.70%, 3.00%, and 7.00%, respectively), suggesting that the comprehensive controlling of dust, motor vehicle emission for green travel, as well as O₃ and VOCs should be the primary focus for future pollution control. The contributions of coal combustion (42.9%) and dust (33.4%) to EPFRs were relatively high on heavy pollution days, whereas the contributions of traffic emission (31.7%) and secondary sources (8.95%) were relatively high on clean days, suggesting that in addition to reduce heavy pollution days, the health impact of EPFRs on clean days also warrant further attention.

Key words： environmentally persistent free radicals(EPFRs) PM_2.5 pollution characteristics source Three-year Action Plan

收稿日期: 2023-03-05

PACS:

X51

基金资助:黄土与第四纪地质国家重点实验室开放基金资助项目（SKLLQG2217）；陕西省基础研究重点项目-科技新星（2021KJXX-36）；陕西省重点研发计划一般项目（2023-YBGY-279）；未央区科技计划项目（202224）

通讯作者: 陈庆彩,教授,chenqingcai@sust.edu.cn E-mail: chenqingcai@sust.edu.cn

作者简介: 丁佳乐(1999-),女,陕西西安人,陕西科技大学硕士研究生,主要研究方向为大气污染及健康效应.dingjiale2021@126.com.

引用本文:

丁佳乐, 陈庆彩, 张梓萌, 韩月梅. “三年行动计划”对大气环境持久性自由基污染特征和来源的影响[J]. 中国环境科学, 2023, 43(10): 5041-5051. DING Jia-le, CHEN Qing-cai, ZHANG Zi-meng, HAN Yue-mei. Effects of the Three-year Action Plan on pollution characteristics and sources of environmentally persistent free radicals in the atmosphere. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(10): 5041-5051.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2023/V43/I10/5041

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