Molecular composition of urban organic aerosols on clear and hazy days in Beijing: a comparative study using FT-ICR MS
Molecular composition of urban organic aerosols on clear and hazy days in Beijing: a comparative study using FT-ICR MS
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北京晴天和雾天城市有机气溶胶的分子组成：基于 FT-ICR MS 的比较研究
DOI：
10.1071/en15230
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发表时间：
2016-07
影响因子：
4.3
通讯作者：
Quan Shi
中科院分区：
文献类型：
--
作者：
Bin Jiang;Bin Yu Kuang;Yongmei Liang;Jingyi Zhang;X. H. Hilda Huang;Chunming Xu;Jian Zhen Yu;Quan Shi
环境背景近年来，中国经历了严重的颗粒物污染和频繁的雾霾事件。利用高分辨质谱技术对北京市晴天和灰霾天有机气溶胶的分子组成进行了比较。对比研究表明，北京城市大气中的氧化、硫酸化和硝化过程都与人为前体物质密切相关。摘要灰霾天气是我国多个城市频繁发生的一种天气现象，严重威胁着人类健康。详细了解二次有机气溶胶的化学组成，为研究灰霾的形成机理及其对人体健康的影响提供了基础资料。在我们的工作中，二氯甲烷和水提取物的环境气溶胶收集在北京的雾霾和晴朗的日子，其特征在于负离子电喷雾电离和傅里叶变换离子回旋共振质谱（FT-ICR MS）。在四个元素组成组，即CHOS，CHONS，CHO和CHON的公式，确定依赖于FT-ICR MS的分辨率和质量准确度。显着更多的化合物被检测到，峰更强烈的浑浊的一天样品，特别是对于CHOS，CHONS和CHON公式组。有机硫酸盐（OS）和硝基氧-有机硫酸盐（硝基氧OS）分别是CHOS和CHONS分子式的主要形式，它们的数量在雾霾天增加了两倍多。在北京严重污染条件下，OS和硝基氧OS的组成分布呈现出明显的特征，如低双键当量（DBE）的强峰（对于OS，DBE=0，1，对于硝基氧基OS，DBE=1，2）和中等DBE的低程度氧化（对于OS，DBE=2，3，对于硝基氧基OS，DBE=3，4）和高DBE（对于OS，DBE ≥ 4，对于硝基氧基OS，DBE ≥ 5）。这些可能的各自的候选人可能是脂肪族OS具有较低的氧化程度，生物源OS和许多芳香族和多环芳烃（PAH）衍生的OS。CHON公式上观察到的有雾的日子是那些在晴朗的日子，有较高的DBE值和较大的O/N比的两倍。在阴天样品中检测到稍微更多的CHO化合物，它们具有更高的DBE值和更多的氧原子。对比研究表明，氧化，硫酸化和硝化过程积极参与北京污染的城市大气中的人为来源的前体。
Environmental context China has been experiencing severe particulate pollution and frequent haze episodes in recent years. We compare the molecular composition of urban organic aerosols on clear and hazy days in Beijing by high-resolution mass spectrometry. The comparative study shows that oxidation, sulfation and nitrification processes actively involve precursors of anthropogenic origin in the Beijing polluted urban atmosphere. Abstract Haze has frequently affected many cities and threatened human health in China. Detailed knowledge of the chemical composition of secondary organic aerosol provides fundamental information in the study of the formation mechanism of haze and its adverse effects on human health. In our work, dichloromethane and water extracts of ambient aerosols collected on hazy and clear days in Beijing were characterised by negative-ion electrospray ionisation and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Formulae in four elemental compositional groups, namely CHOS, CHONS, CHO and CHON, were identified relying on the ultrahigh resolution and mass accuracy of FT-ICR MS. Significantly more compounds were detected and the peaks were much more intense in the hazy day samples, especially for the CHOS, CHONS and CHON formula groups. Organosulfates (OS) and nitrooxy-organosulfates (nitrooxy OS) were the major forms of CHOS and CHONS formulae respectively, and their numbers more than tripled on the hazy days. Under the severely polluted conditions in Beijing, the compositional distribution of the OS and nitrooxy OS exhibited distinct features such as intense peaks of low double-bond equivalent (DBE) (DBE=0, 1 for OS and DBE=1, 2 for nitrooxy OS) and low degree oxidation, of medium DBE (DBE=2, 3 for OS and DBE=3, 4 for nitrooxy OS), and of high DBE (DBE ≥ 4 for OS and DBE ≥ 5 for nitrooxy OS). The likely respective candidates for these could be aliphatic OS having a low degree of oxidation, biogenic OS and many aromatics and polycyclic aromatic hydrocarbon (PAH)-derived OS. The CHON formulae observed on hazy days were double those on clear days and had higher DBE values and larger O/N ratios. Slightly more CHO compounds were detected in the hazy-day samples and they had higher DBE values and more oxygen atoms. The comparative study suggests that oxidation, sulfation and nitrification processes actively involve precursors of anthropogenic origin in the Beijing polluted urban atmosphere.
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影响因子：
2
作者：
Anil Kumar Yadav;Krishan Kumar;Awg Makarimi bin Hj Awg Kasim-Awg-Makarimi-bin-Hj-Awg-Kasim-104749359;M. P. Singh;S. Parida;Maithili Sharan
通讯作者：
Anil Kumar Yadav;Krishan Kumar;Awg Makarimi bin Hj Awg Kasim-Awg-Makarimi-bin-Hj-Awg-Kasim-104749359;M. P. Singh;S. Parida;Maithili Sharan
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影响因子：
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