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首页> 外文期刊>Environmental Science & Technology >Formation and Optical Properties of Brown Carbon from Small α-Dicarbonyls and Amines
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Formation and Optical Properties of Brown Carbon from Small α-Dicarbonyls and Amines

机译：小α-二羰基和胺类化合物形成棕碳的性质和光学性质

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摘要

Brown Carbon (BrC) aerosols scatter and absorb solar radiation, directly affecting the Earth's radiative budget. However, considerable uncertainty exists concerning the chemical mechanism leading to BrC formation and their optical properties. In this work, BrC particles were prepared from mixtures of small alpha-dicarbonyls (glyoxal and methylglyoxal) and amines (methylamine, dimethylamine, and trimethylamine). The absorption and scattering of BrC particles were measured using a photoacoustic extinctometer (405 and 532 nm), and the chemical composition of the alpha-dicarbonyl-amine mixtures was analyzed using orbitrap-mass spectrometry and thermal desorption-ion drift-chemical ionization mass spectrometry. The single scattering albedo for methylglyoxal-amine mixtures is smaller than that of glyoxal-amine mixtures and increases with the methyl substitution of amines. The mass absorption cross-section for methylglyoxal-amine mixtures is two times higher at 405 nm wavelength than that at 532 nm wavelength. The derived refractive indexes at the 405 nm wavelength are 1.40-1.64 for the real part and 0.002-0.195 for the imaginary part. Composition analysis in the alpha-dicarbonyl-amine mixtures reveals N-heterocycles as the dominant products, which are formed via multiple steps involving nucleophilic attack, steric hindrance, and dipole dipole interaction between alpha-dicarbonyls and amines. BrC aerosols, if formed from the particle-phase reaction of methylglyoxal with methylamine, likely contribute to atmospheric warming.
机译：褐碳（BrC）气溶胶会散射并吸收太阳辐射，直接影响地球的辐射预算。然而，关于导致BrC形成的化学机理及其光学性质存在很大的不确定性。在这项工作中，BrC颗粒是由小的α-二羰基（乙二醛和甲基乙二醛）和胺（甲胺，二甲胺和三甲胺）的混合物制得的。使用光声消光仪（405和532 nm）测量BrC颗粒的吸收和散射，并使用轨道阱质谱和热解吸-离子漂移-化学电离质谱法分析α-二羰基-胺混合物的化学成分。甲基乙二醛-胺混合物的单次散射反照率小于乙二醛-胺混合物的单次散射，并随胺的甲基取代而增加。甲基乙二醛-胺混合物的质量吸收截面在405 nm波长处是在532 nm波长处的两倍。在405 nm波长处导出的折射率，实部为1.40-1.64，虚部为0.002-0.195。在α-二羰基-胺混合物中的成分分析表明，N-杂环是主要产物，它是通过多个步骤形成的，这些步骤涉及亲核攻击，位阻以及α-二羰基和胺之间的偶极偶极相互作用。如果BrC气溶胶是由甲基乙二醛与甲胺的颗粒相反应形成的，则可能会导致大气变暖。

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  • 来源
    《Environmental Science & Technology》 |2019年第1期|117-126|共10页
  • 作者

    Marrero-Ortiz Wilmarie; Hu Min; Du Zhuofei; Ji Yuemeng; Wang Yujue; Guo Song; Lin Yun; Gomez-Hermandez Mario; Peng Jianfei; Li Yixin; Secrest Jeremiah; Zamora Misti L.; Wang Yuan; An Taicheng; Zhang Renyi;

  • 作者单位

    Texas A&M Univ, Dept Chem, College Stn, TX 77840 USA;

    Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China;

    Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China;

    Nankai Univ, Coll Environm Sci & Engn, Ctr Urban Transport Emiss Res, Tianjin 300071, Peoples R China|Nankai Univ, Coll Environm Sci & Engn, State Environm Protect Key Lab Urban Ambient Air, Tianjin 300071, Peoples R China|Guangdong Univ Technol, Sch Environm Sci & Engn,Inst Environm Hlth & Poll, Guangdong Key Lab Environm Catalysis & Hlth Risk, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510006, Guangdong, Peoples R China;

    Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China;

    Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China;

    Texas A&M Univ, Dept Atmospher Sci, College Stn, TX 77843 USA;

    Texas A&M Univ, Dept Chem, College Stn, TX 77840 USA|Florida Int Univ, Dept Chem & Biochem, Miami, FL 33199 USA;

    Texas A&M Univ, Dept Atmospher Sci, College Stn, TX 77843 USA;

    Texas A&M Univ, Dept Chem, College Stn, TX 77840 USA;

    Texas A&M Univ, Dept Chem, College Stn, TX 77840 USA;

    Texas A&M Univ, Dept Atmospher Sci, College Stn, TX 77843 USA|Johns Hopkins Univ, Johns Hopkins Sch Publ Hlth, Environm Hlth & Engn, Baltimore, MD 21218 USA;

    CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USA;

    Guangdong Univ Technol, Sch Environm Sci & Engn,Inst Environm Hlth & Poll, Guangdong Key Lab Environm Catalysis & Hlth Risk, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510006, Guangdong, Peoples R China;

    Texas A&M Univ, Dept Chem, College Stn, TX 77840 USA|Texas A&M Univ, Dept Atmospher Sci, College Stn, TX 77843 USA;

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