色谱 ›› 2019, Vol. 37 ›› Issue (6): 634-643.DOI: 10.3724/SP.J.1123.2018.12012

• 研究论文 • 上一篇    下一篇

替代模板印迹-高效液相色谱测定空气PM2.5中的羰基化合物

方思炀1, 陈诗丽1, 何嘉铧1, 王浩1, 沈丽思1, 刘洋洋1, 孙慧1,3, 赖家平2   

  1. 1. 广州大学环境科学与工程学院, 广东 广州 510006;
    2. 华南师范大学化学与环境学院, 广东 广州 510006;
    3. 广东省放射性核素污染控制以及资源化重点实验室, 广东 广州 510006
  • 收稿日期:2018-12-09 出版日期:2019-06-08 发布日期:2015-04-17
  • 通讯作者: 孙慧,E-mail:esesunhui@gzhu.edu.cn;赖家平,E-mail:laijp@scnu.edu.cn.
  • 基金资助:

    国家自然科学基金(21477026,21677053,21876033);广州市科技计划项目(201607010295);广州大学大学生创新训练项目(201711078061).

Determination of carbonyls in ambient PM2.5 by coupling dummy template imprinting technology and high performance liquid chromatography

FANG Siyang1, CHEN Shili1, HE Jiahua1, WANG Hao1, SHEN Lisi1, LIU Yangyang1, SUN Hui1,3, LAI Jiaping2   

  1. 1. School of Environmental Science & Engineering, Guangzhou University, Guangzhou 510006, China;
    2. School of Chemistry & Environment, South China Normal University, Guangzhou 510006, China;
    3. Guangdong Provincial Key Laboratory of Radionuclides Pollution Control and Resources, Guangzhou 510006, China
  • Received:2018-12-09 Online:2019-06-08 Published:2015-04-17
  • Supported by:

    National Natural Science Foundation of China (Nos. 21477026, 21677053, 21876033); Guangzhou Science and Technology Project (No. 201607010295); the Undergraduate Innovation Training Project of Guangzhou University (No. 201711078061).

摘要:

以替代模板法制备了分子印迹固相萃取柱(MISPE),该柱能够有效去除空气PM2.5样品分析过程中过量的衍生剂2,4-二硝基苯肼(2,4-DNPH),并能够大幅度浓缩样品溶液,提高羰基化合物的富集效率和监测灵敏度,缩短采样时间。与高效液相色谱联用,实现了对空气PM2.5中的羰基化合物的快速检测。本研究解决了传统固相萃取材料选择性低,不能去除2,4-DNPH干扰的瓶颈问题。本方法用于研究广州市大学城早春季节雾霾天和非霾天羰基化合物水平及其来源,结果发现无论是灰霾天气还是正常天气,14种目标羰基化合物均被检出。研究发现,在污染物排放和天气因素的影响下,灰霾天气羰基化合物总量增高,尤其是异戊醛增长迅速,并且与丙醛浓度变化呈现高度正相关。通过相关性分析,证明除了光化学反应等自然因素,人类活动对广州羰基化合物水平的干扰严重,应引起重视。

关键词: PM2.5, 分子印迹聚合物, 高效液相色谱, 固相萃取, 空气, 羰基化合物

Abstract:

The determination of ambient carbonyls by the derivative method inevitably leads to the introduction of extra 2,4-dinitrophenylhydrazine (2,4-DNPH) into the sample solution. Traditional solid phase extraction (SPE) materials cannot remove this interference. To address this issue, a selective molecularly imprinted solid phase extraction (MISPE) column was prepared. With 2,4-dinitroaniline (2,4-DNAN) as the dummy template, MISPE could eliminate the excessive derivative agent (2,4-DNPH) in the air samples. Consequently, the sample could be concentrated effectively while the sensitivity increased greatly. By coupling MISPE and high performance liquid chromatography (HPLC), the developed method was used to study the concentration and source of 14 carbonyls of PM2.5 during spring in Guangzhou Higher Education Mega Center. Results showed that the total concentration of carbonyls increased with the level of air pollution. Particularly, the content of isovaleraldehyde increased sharply to account for 21% of the 14 total carbonyls in the haze days. Moreover, a high positive correlation between isovaleraldehyde and propionaldehyde was found either in normal days or haze days. From the correlation analysis, it was shown that anthropogenic emissions together with photochemical reaction had contributed to the abnormally high levels of carbonyls in ambient PM2.5 in the haze days. This aspect should be further investigated.

Key words: air, carbonyls, high performance liquid chromatography (HPLC), molecularly imprinted polymer (MIP), PM2.5, solid phase extraction (SPE)

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