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大气细颗粒物中类腐殖酸类化合物的有效毒性组分的筛选和鉴定

批准号:
42077197
项目类别:
面上项目
资助金额:
57.0 万元
负责人:
马慧敏
学科分类:
环境大气科学
结题年份:
2024
批准年份:
2020
项目状态:
已结题
项目参与者:
马慧敏

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中文摘要
大气细颗粒物中有效毒性组分的筛选和鉴定是环境大气化学领域的关键科学问题。最新的研究发现,细颗粒物中有机碳的主要成分类腐殖酸类化合物(Humic-like Substances HULIS)对人体心肺健康有显著危害,但是由于近期才被关注,HULIS诱导的毒性特点,及有效毒性组分的结构、组成和来源特征尚缺乏系统研究。本研究基于前期对大气HULIS的毒性研究的基础,针对不同典型排放源PM2.5中的HULIS样品,利用人体肺细胞模型,分析其毒性差异和剂量效应关系,及其主要信号通路,并利用核磁共振(NMR),超高分辨质谱(FT-ICR MS),分析有效毒性组分的结构组成信息,结论在真实大气中做进一步验证,利用加速器质谱(AMS)等技术进行源解析,探索筛选HULIS中有效毒性组分的结构组成信息和源信息。结论可以为优化大气污染物的排放标准提供关键数据,并为大气颗粒物的精准治疗和预防提供精确靶点。
英文摘要
The screening of effective toxic components in fine particles is a key scientific problem in the field of atmospheric environmental chemistry. The latest research found that the harm of Humic-Like Substances (HULIS), the main component of organic carbon in fine particles, to human health cannot be ignored. But because of the recent attention, the toxicity characteristics induced by HULIS, and the structure, composition and source characteristics of effective toxic components are still lack of systematic research. Based on our previous study on the toxicity of HULIS, this study analyzed the toxicity difference, dose effect relationship and special pathway of HULIS in PM2.5 of different emission sources by using human lung cell model, what’s more, using Nuclear Magnetic Resonance(NMR), Fourier-transform ion cyclotron resonance-mass spectrometer(FT-ICR MS), and other technologies to analyze the structure and composition information of effective toxic components of HULIS. The results will be further analyzed and validated in the real atmospheric samples (HULIS samples of PM2.5 in Guangzhou urban and suburb during one year). The toxicity changes of HULIS in different seasons and regions and the differences of its signal pathways were analyzed. The source information of HULIS in Guangzhou urban and suburb was analyzed by accelerator mass spectrometry (AMS) to verify the contribution of different emission sources to toxicity. The structure and composition characteristics of the effect toxic components of HULIS was analyzed and identified. The conclusion of this project can provide key data for the establishment of emission standards of air pollutants, and provide accurate targets for the precise treatment and prevention of atmospheric particles.
大气细颗粒物(PM2.5)污染对人体健康的危害日益受到关注,其中类腐殖酸物质(HULIS)作为PM2.5中有机碳的主要成分,其毒性组分鉴定与来源解析是环境健康研究的关键科学问题。本研究系统采集交通源、生物质燃烧源、燃煤源等19类PM2.5典型排放样品及广州市环境样本,结合高分辨质谱(FT-ICR MS)、核磁共振(NMR)、细胞毒理学及同位素源解析技术,揭示了HULIS的有效毒性组分及其作用机制。研究首次从HULIS中筛选出硝基多环芳烃(Nitro-PACs)等12类关键毒性化合物,其中含氮化合物(CHON类)占比36.8%,C14H9NO4(二硝基蒽)和C20H11NO3(硝基苯并[a]芘)的凋亡贡献率分别达21.3%和15.7%,分子双键等效数(DBE≥14)与凋亡率显著正相关(r=0.72,p<0.01)。源解析结果显示,生物质燃烧(34.5±6.2%)和燃煤(28.1±5.8%)是HULIS的主要来源,冬季二次硝酸盐生成的贡献率达42.7%,柴油车低速工况(<30 km/h)下PM2.5有机组分的凋亡活性较高速工况显著升高(15.8% vs. 6.3%)。毒性机制上,HULIS通过线粒体途径(Caspase-3活性升高4.3倍)与死亡受体通路(FasL表达上调2.8倍)协同诱导肺细胞凋亡,并发现AhR基因启动子区低甲基化(Δβ=-0.18,p=0.008)的表观遗传特征。项目融合环境化学与毒理学方法,提出生物质燃烧与燃煤源毒性组分的优先管控建议,共发表SCI论文3篇(含环境领域顶刊ES&T1篇),培养博士2名,为我国大气污染精准治理提供了科学支撑。
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