Parameterized Yields of Semivolatile Products from Isoprene Oxidation under Different NO Levels: Impacts of Chemical Aging and Wall-Loss of Reactive Gases

被引:2
作者
Xing, Li [1 ,2 ,3 ,4 ]
Shrivastava, Manish [3 ]
Fu, Tzung-May [1 ,2 ]
Roldin, Pontus [5 ]
Qian, Yun [3 ]
Xu, Lu [6 ,7 ]
Ng, Nga L. [6 ,8 ]
Shilling, John [3 ]
Zelenyuk, Alla [3 ]
Cappa, Christopher D. [9 ]
机构
[1] Peking Univ, Dept Atmospher & Ocean Sci, Sch Phys, Beijing 100871, Peoples R China
[2] Peking Univ, Sch Phys, Lab Climate & Ocean Atmosphere Studies, Beijing 100871, Peoples R China
[3] Pacific Northwest Natl Lab, Washington, DC 99352 USA
[4] Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol, Key Lab Aerosol Chem & Phys, Xian 710061, Shaanxi, Peoples R China
[5] Lund Univ, Div Nucl Phys, POB 118, S-22100 Lund, Sweden
[6] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[7] Georgia Inst Technol, Div Geol & Planetary Sci, Pasadena, CA 91125 USA
[8] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[9] Univ Calif Davis, Dept Civil & Environm Engn, Davis, CA 95616 USA
基金
美国国家科学基金会; 中国国家自然科学基金;
关键词
SECONDARY ORGANIC AEROSOL; VOLATILITY BASIS-SET; PHASE FRAGMENTATION REACTIONS; SIZE DISTRIBUTION DYNAMICS; TRANSPORT MODEL; PHOTOOXIDATION; EVOLUTION; SOA; CHAMBER; GROWTH;
D O I
10.1021/acs.est.8b00373
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NOx levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NOx-sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NOx levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box model can be expanded to include more explicit chemical aging processes and help ultimately bridge the gap between the process based understanding of SOA formation from VOC oxidation and the bulk-yield parametrizations used in chemical transport models.
引用
收藏
页码:9225 / 9234
页数:10
相关论文
共 54 条
  • [1] A volatility basis set model for summertime secondary organic aerosols over the eastern United States in 2006
    Ahmadov, R.
    McKeen, S. A.
    Robinson, A. L.
    Bahreini, R.
    Middlebrook, A. M.
    de Gouw, J. A.
    Meagher, J.
    Hsie, E-Y
    Edgerton, E.
    Shaw, S.
    Trainer, M.
    [J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2012, 117
  • [2] RATE CONSTANTS FOR THE REACTION OF OH RADICALS WITH A SERIES OF ALKENES AND DIALKENES AT 295 +/- 1-K
    ATKINSON, R
    ASCHMANN, SM
    [J]. INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1984, 16 (10) : 1175 - 1186
  • [3] Gas Phase Production and Loss of Isoprene Epoxydiols
    Bates, Kelvin H.
    Crounse, John D.
    St Clair, Jason M.
    Bennett, Nathan B.
    Nguyen, Tran B.
    Seinfeld, John H.
    Stoltz, Brian M.
    Wennberg, Paul O.
    [J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2014, 118 (07) : 1237 - 1246
  • [4] Multi-generation gas-phase oxidation, equilibrium partitioning, and the formation and evolution of secondary organic aerosol
    Cappa, C. D.
    Wilson, K. R.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (20) : 9505 - 9528
  • [5] Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior
    Cappa, C. D.
    Wilson, K. R.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (05) : 1895 - 1911
  • [6] Simulating secondary organic aerosol in a regional air quality model using the statistical oxidation model - Part 2: Assessing the influence of vapor wall losses
    Cappa, Christopher D.
    Jathar, Shantanu H.
    Kleeman, Michael J.
    Docherty, Kenneth S.
    Jimenez, Jose L.
    Seinfeld, John H.
    Wexler, Anthony S.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2016, 16 (05) : 3041 - 3059
  • [7] Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NOx conditions
    D'Ambro, Emma L.
    Lee, Ben H.
    Liu, Jiumeng
    Shilling, John E.
    Gaston, Cassandra J.
    Lopez-Hilfiker, Felipe D.
    Schobesberger, Siegfried
    Zaveri, Rahul A.
    Mohr, Claudia
    Lutz, Anna
    Zhang, Zhenfa
    Gold, Avram
    Surratt, Jason D.
    Rivera-Rios, Jean C.
    Keutsch, Frank N.
    Thornton, Joel A.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2017, 17 (01) : 159 - 174
  • [8] A two-dimensional volatility basis set - Part 2: Diagnostics of organic-aerosol evolution
    Donahue, N. M.
    Kroll, J. H.
    Pandis, S. N.
    Robinson, A. L.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (02) : 615 - 634
  • [9] A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics
    Donahue, N. M.
    Epstein, S. A.
    Pandis, S. N.
    Robinson, A. L.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (07) : 3303 - 3318
  • [10] Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions
    Donahue, Neil M.
    Henry, Kaytlin M.
    Mentel, Thomas F.
    Kiendler-Scharr, Astrid
    Spindler, Christian
    Bohn, Birger
    Brauers, Theo
    Dorn, Hans P.
    Fuchs, Hendrik
    Tillmann, Ralf
    Wahner, Andreas
    Saathoff, Harald
    Naumann, Karl-Heinz
    Moehler, Ottmar
    Leisner, Thomas
    Mueller, Lars
    Reinnig, Marc-Christopher
    Hoffmann, Thorsten
    Salo, Kent
    Hallquist, Mattias
    Frosch, Mia
    Bilde, Merete
    Tritscher, Torsten
    Barmet, Peter
    Praplan, Arnaud P.
    DeCarlo, Peter F.
    Dommen, Josef
    Prevot, Andre S. H.
    Baltensperger, Urs
    [J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (34) : 13503 - 13508