...
首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Reactive intermediates revealed in secondary organic aerosol formation from isoprene
【24h】

Reactive intermediates revealed in secondary organic aerosol formation from isoprene

机译:异戊二烯二次有机气溶胶形成过程中发现的反应性中间体

获取原文
获取原文并翻译 | 示例
           

摘要

Isoprene is a significant source of atmospheric organic aerosol; however, the oxidation pathways that lead to secondary organic aerosol (SOA) have remained elusive. Here, we identify the role of two key reactive intermediates, epoxydiols of isoprene (IEPOX = β-IEPOX + δ- IEPOX) and methacryloylperoxynitrate (MPAN), which are formed during isoprene oxidation under low- and high-NO_x conditions, respectively. Isoprene low-NO_x SOA is enhanced in the presence of acidified sulfate seed aerosol (mass yield 28.6%) over that in the presence of neutral aerosol (mass yield 1.3%). Increased uptake of IEPOX by acid-catalyzed particle-phase reactions is shown to explain this enhancement. Under high-NO_x conditions, isoprene SOA formation occurs through oxidation of its second-generation product, MPAN. The similarity of the composition of SOA formed from the photooxidation of MPAN to that formed from isoprene and methacrolein demonstrates the role of MPAN in the formation of isoprene high-NO_x SOA. Reactions of IEPOX and MPAN in the presence of anthropogenic pollutants (i.e., acidic aerosol produced from the oxidation of SO_2 and NO_2, respectively) could be a substantial source of "missing urban SOA" not included in current atmospheric models.
机译:异戊二烯是大气中有机气溶胶的重要来源。但是,导致二次有机气溶胶(SOA)的氧化途径仍然难以捉摸。在这里,我们确定了两种关键的反应中间体的作用,异戊二烯的环氧二醇(IEPOX =β-IEPOX+δ-IEPOX)和甲基丙烯酰过氧硝酸盐(MPAN),它们分别在低和高NO_x条件下的异戊二烯氧化过程中形成。在存在酸化的硫酸盐种子气溶胶(质量产率为28.6%)的情况下,异戊二烯低NO_x SOA的浓度要比在中性气溶胶存在的质量浓度为1.3%的情况下有所提高。结果表明,酸催化的颗粒相反应增加了IEPOX的吸收,可以解释这种增强。在高NOxx条件下,异戊二烯SOA的形成通过其第二代产物MPAN的氧化而发生。由MPAN的光氧化形成的SOA组成与由异戊二烯和甲基丙烯醛形成的SOA组成相似,证明了MPAN在形成异戊二烯高NO_x SOA中的作用。在人为污染物(即分别由SO_2和NO_2氧化产生的酸性气溶胶)存在下,IEPOX和MPAN的反应可能是当前大气模型中未包括的“缺少城市SOA”的重要来源。

著录项

  • 来源
  • 作者单位

    Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125;

    Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125;

    Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125;

    Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125;

    Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125;

    Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125;

    Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125;

    Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125 Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125;

    Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125 Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125;

    Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125 Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125;

  • 收录信息 美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    acid-catalyzed particle-phase reactions; epoxides methacryloylperoxynitrate; organosulfates;

    机译:酸催化的颗粒相反应;环氧甲基丙烯酰过氧硝酸盐;有机硫酸盐;

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱:kefu@zhangqiaokeyan.com

京公网安备:11010802029741号 ICP备案号:京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有
  • 客服微信

  • 服务号