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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer
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Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer

机译:大气边界层污染成核速率的酸碱化学反应模型

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摘要

Climate models show that particles formed by nucleation can affect cloud cover and, therefore, the earth's radiation budget. Measurements worldwide show that nucleation rates in the atmospheric boundary layer are positively correlated with concentrations of sulfuric acid vapor. However, current nucleation theories do not correctly predict either the observed nucleation rates or their functional dependence on sulfuric acid concentrations. This paper develops an alternative approach for modeling nucleation rates, based on a sequence of acid-base reactions. The model uses empirical estimates of sulfuric acid evaporation rates obtained from new measurements of neutral molecular clusters. The model predicts that nucleation rates equal the sulfuric acid vapor collision rate times a prefactor that is less than unity and that depends on the concentrations of basic gaseous compounds and preexisting particles. Predicted nucleation rates and their dependence on sulfuric acid vapor concentrations are in reasonable agreement with measurements from Mexico City and Atlanta.
机译:气候模型表明,由成核作用形成的颗粒会影响云层覆盖,从而影响地球的辐射预算。全世界的测量表明,大气边界层中的成核速率与硫酸蒸气的浓度成正相关。但是,当前的成核理论不能正确预测观察到的成核速率或它们对硫酸浓度的功能依赖性。本文基于一系列酸碱反应,开发了一种用于模拟成核速率的替代方法。该模型使用从对中性分子簇的新测量中获得的硫酸蒸发速率的经验估计。该模型预测成核速率等于硫酸蒸气碰撞速率乘以小于1的因子,该因子取决于碱性气体化合物和预先存在的颗粒的浓度。预测的成核速率及其对硫酸蒸气浓度的依赖性与墨西哥城和亚特兰大的测量结果合理吻合。

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  • 作者单位

    Departments of Mechanical Engineering, Minneapolis, MN 55455;

    Departments of Chemistry, University of Minnesota, Minneapolis, MN 55455,Environmental Program, Colorado College, Colorado Springs, CO 80206;

    Departments of Mechanical Engineering, Minneapolis, MN 55455,State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China;

    Departments of Mechanical Engineering, Minneapolis, MN 55455;

    Atmospheric Sciences Division, Brookhaven National Laboratory, Upton, NY 11973;

    Sustainable Energy Systems Group, Environmental Energy Technologies Division, E. O. Lawrence Berkeley National Laboratory, Berkeley, CA 94720;

    Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, CO 80307;

    Departments of Chemistry, University of Minnesota, Minneapolis, MN 55455;

    Chemistry Department, Augsburg College, Minneapolis, MN 55455;

    Departments of Mechanical Engineering, Minneapolis, MN 55455;

    Departments of Mechanical Engineering, Minneapolis, MN 55455;

  • 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

    amines; atmospheric aerosol; climate forcing; nanoparticle; chamber study;

    机译:胺;大气气溶胶气候强迫;纳米粒子室研究;

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