Photo-oxidation of Aromatic Hydrocarbons Produces Low-Volatility Organic Compounds.,Environmental Science & Technology

当前位置： X-MOL 学术 › Environ. Sci. Technol. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Photo-oxidation of Aromatic Hydrocarbons Produces Low-Volatility Organic Compounds.
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-06-09 , DOI: 10.1021/acs.est.0c02100
Mingyi Wang _{1,

2} , Dexian Chen _{1,

3} , Mao Xiao ₄ , Qing Ye _{1,

2} , Dominik Stolzenburg ₅ , Victoria Hofbauer _{1,

2} , Penglin Ye ₆ , Alexander L Vogel ₇ , Roy L Mauldin _{1,

2,

8} , Antonio Amorim ₉ , Andrea Baccarini ₄ , Bernhard Baumgartner ₅ , Sophia Brilke ₅ , Lubna Dada ₁₀ , António Dias ₉ , Jonathan Duplissy _{10,

11} , Henning Finkenzeller ₁₂ , Olga Garmash ₁₀ , Xu-Cheng He ₁₀ , Christopher R Hoyle _{4,

13} , Changhyuk Kim _{14,

15} , Alexander Kvashnin ₁₆ , Katrianne Lehtipalo _{10,

17} , Lukas Fischer ₁₈ , Ugo Molteni ₄ , Tuukka Petäjä ₁₀ , Veronika Pospisilova ₄ , Lauriane L J Quéléver ₁₀ , Matti Rissanen ₁₉ , Mario Simon ₇ , Christian Tauber ₅ , António Tomé ₂₀ , Andrea C Wagner _{7,

12} , Lena Weitz ₇ , Rainer Volkamer ₁₂ , Paul M Winkler ₅ , Jasper Kirkby _{7,

21} , Douglas R Worsnop _{6,

10} , Markku Kulmala _{10,

11,

22,

23} , Urs Baltensperger ₄ , Josef Dommen ₄ , Imad El-Haddad ₄ , Neil M Donahue _{1,

2,

3,

24}

Affiliation

Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.
Department of Chemistry, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.
Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
Aerodyne Research, Incorporated, Billerica, Massachusetts 01821, United States.
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438, Frankfurt am Main, Germany.
Department of Oceanic and Atmospheric Science, University of Colorado Boulder, Boulder, Colorado 80309, United States.
CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal.
Institute for Atmospheric and Earth System Research (INAR), University of Helsinki, 00014 Helsinki, Finland.
Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland.
Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, Colorado 80309, United States.
Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich, Switzerland.
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States.
Department of Environmental Engineering, Pusan National University, Busan, 46241, Republic of Korea.
Lebedev Physical Institute, 119991 Moscow, Russia.
Finnish meteorological Institute, Erik Palménin aukio 1, 00560 Helsinki, Finland.
Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
Aerosol Physics Laboratory, Physics Unit, Tampere University, P.O. Box 1001, Tampere 33100, Finland.
IDL-University of Beira Interior, Covilhã 6201-001, Portugal.
CERN, 1211 Geneva, Switzerland.
Joint International Research Laboratory of Atmospheric and Earth System Sciences, Nanjing University, Nanjing 210044, P. R. China.
Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China.
Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.

To better understand the role of aromatic hydrocarbons in new-particle formation, we measured the particle-phase abundance and volatility of oxidation products following the reaction of aromatic hydrocarbons with OH radicals. For this we used thermal desorption in an iodide-adduct Time-of-Flight Chemical-Ionization Mass Spectrometer equipped with a Filter Inlet for Gases and AEROsols (FIGAERO-ToF-CIMS). The particle-phase volatility measurements confirm that oxidation products of toluene and naphthalene can contribute to the initial growth of newly formed particles. Toluene-derived (C₇) oxidation products have a similar volatility distribution to that of α-pinene-derived (C₁₀) oxidation products, while naphthalene-derived (C₁₀) oxidation products are much less volatile than those from toluene or α-pinene; they are thus stronger contributors to growth. Rapid progression through multiple generations of oxidation is more pronounced in toluene and naphthalene than in α-pinene, resulting in more oxidation but also favoring functional groups with much lower volatility per added oxygen atom, such as hydroxyl and carboxylic groups instead of hydroperoxide groups. Under conditions typical of polluted urban settings, naphthalene may well contribute to nucleation and the growth of the smallest particles, whereas the more abundant alkyl benzenes may overtake naphthalene once the particles have grown beyond the point where the Kelvin effect strongly influences the condensation driving force.

中文翻译：

芳烃的光氧化产生低挥发性有机化合物。

为了更好地理解芳烃在新颗粒形成中的作用，我们测量了芳烃与OH自由基反应后颗粒相的丰度和氧化产物的挥发性。为此，我们在配备有气体和气溶胶过滤器入口的碘化物加合物飞行时间化学电离质谱仪中使用了热脱附技术（FIGAERO-ToF-CIMS）。颗粒相挥发性测量结果证实，甲苯和萘的氧化产物可有助于新形成颗粒的初始生长。甲苯衍生的（C ₇）氧化产物的挥发性分布与α-pine烯衍生的（C ₁₀）氧化产物相似，而萘衍生的（C ₁₀）氧化产物的挥发性比甲苯或α-pine烯的低。因此，它们是促进增长的强大力量。与α-pine烯相比，甲苯和萘通过多代氧化的快速进展更为明显，从而导致更多的氧化反应，但同时也有利于每添加一个氧原子具有较低挥发性的官能团，例如羟基和羧基而不是氢过氧化物基团。在典型的城市环境污染条件下，萘可能有助于成核和最小颗粒的生长，而一旦颗粒生长超过开尔文效应强烈影响缩合驱动力的程度，则更丰富的烷基苯可能会取代萘。

更新日期：2020-07-07

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11