Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions

被引:213
作者
Donahue, Neil M. [1 ]
Henry, Kaytlin M. [1 ]
Mentel, Thomas F. [2 ]
Kiendler-Scharr, Astrid [2 ]
Spindler, Christian [2 ]
Bohn, Birger [2 ]
Brauers, Theo [2 ]
Dorn, Hans P. [2 ]
Fuchs, Hendrik [2 ]
Tillmann, Ralf [2 ]
Wahner, Andreas [2 ]
Saathoff, Harald [3 ]
Naumann, Karl-Heinz [3 ]
Moehler, Ottmar [3 ]
Leisner, Thomas [3 ]
Mueller, Lars [4 ]
Reinnig, Marc-Christopher [4 ]
Hoffmann, Thorsten [4 ]
Salo, Kent [5 ]
Hallquist, Mattias [5 ]
Frosch, Mia [6 ]
Bilde, Merete [6 ]
Tritscher, Torsten [7 ]
Barmet, Peter [7 ]
Praplan, Arnaud P. [7 ]
DeCarlo, Peter F. [7 ]
Dommen, Josef [7 ]
Prevot, Andre S. H. [7 ]
Baltensperger, Urs [7 ]
机构
[1] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15217 USA
[2] Forschungszentrum Julich, Inst Energy & Climate Res, D-52425 Julich, Germany
[3] Karlsruhe Inst Technol, Inst Meteorol & Climate Res Atmospher Aerosol Res, D-76021 Karlsruhe, Germany
[4] Johannes Gutenberg Univ Mainz, Inst Organ & Analyt Chem, D-55128 Mainz, Germany
[5] Univ Gothenburg, Dept Chem, SE-41296 Gothenburg, Sweden
[6] Univ Copenhagen, Dept Chem, DK-21000 Copenhagen, Denmark
[7] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland
基金
瑞典研究理事会; 瑞士国家科学基金会;
关键词
atmospheric chemistry; biosphere-atmosphere interactions; VOLATILITY BASIS-SET; ALPHA-PINENE; MASS-SPECTROMETER; PINONIC ACID; CHEMISTRY; OZONOLYSIS; CHAMBER; EMISSIONS; OXIDATION; KINETICS;
D O I
10.1073/pnas.1115186109
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The Multiple Chamber Aerosol Chemical Aging Study (MUCHACHAS) tested the hypothesis that hydroxyl radical (OH) aging significantly increases the concentration of first-generation biogenic secondary organic aerosol (SOA). OH is the dominant atmospheric oxidant, and MUCHACHAS employed environmental chambers of very different designs, using multiple OH sources to explore a range of chemical conditions and potential sources of systematic error. We isolated the effect of OH aging, confirming our hypothesis while observing corresponding changes in SOA properties. The mass increases are consistent with an existing gap between global SOA sources and those predicted in models, and can be described by a mechanism suitable for implementation in those models.
引用
收藏
页码:13503 / 13508
页数:6
相关论文
共 53 条
[1]   Aerosol volatility measurement using an improved thermodenuder: Application to secondary organic aerosol [J].
An, Woo Jin ;
Pathak, Ravi K. ;
Lee, Byong-Hyoek ;
Pandis, Spyros N. .
JOURNAL OF AEROSOL SCIENCE, 2007, 38 (03) :305-314
[2]   Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol [J].
Asa-Awuku, A. ;
Engelhart, G. J. ;
Lee, B. H. ;
Pandis, S. N. ;
Nenes, A. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (03) :795-812
[3]   Gas-phase tropospheric chemistry of volatile organic compounds .1. Alkanes and alkenes [J].
Atkinson, R .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1997, 26 (02) :215-290
[4]   Functionalization vs. fragmentation: n-aldehyde oxidation mechanisms and secondary organic aerosol formation [J].
Chacon-Madrid, Heber J. ;
Presto, Albert A. ;
Donahue, Neil M. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2010, 12 (42) :13975-13982
[5]   Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer [J].
DeCarlo, Peter F. ;
Kimmel, Joel R. ;
Trimborn, Achim ;
Northway, Megan J. ;
Jayne, John T. ;
Aiken, Allison C. ;
Gonin, Marc ;
Fuhrer, Katrin ;
Horvath, Thomas ;
Docherty, Kenneth S. ;
Worsnop, Doug R. ;
Jimenez, Jose L. .
ANALYTICAL CHEMISTRY, 2006, 78 (24) :8281-8289
[6]   A two-dimensional volatility basis set - Part 2: Diagnostics of organic-aerosol evolution [J].
Donahue, N. M. ;
Kroll, J. H. ;
Pandis, S. N. ;
Robinson, A. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (02) :615-634
[7]   A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics [J].
Donahue, N. M. ;
Epstein, S. A. ;
Pandis, S. N. ;
Robinson, A. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (07) :3303-3318
[8]   Evaluation of recently-proposed secondary organic aerosol models for a case study in Mexico City [J].
Dzepina, K. ;
Volkamer, R. M. ;
Madronich, S. ;
Tulet, P. ;
Ulbrich, I. M. ;
Zhang, Q. ;
Cappa, C. D. ;
Ziemann, P. J. ;
Jimenez, J. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (15) :5681-5709
[9]   Relating cloud condensation nuclei activity and oxidation level of α-pinene secondary organic aerosols [J].
Frosch, M. ;
Bilde, M. ;
DeCarlo, P. F. ;
Juranyi, Z. ;
Tritscher, T. ;
Dommen, J. ;
Donahue, N. M. ;
Gysel, M. ;
Weingartner, E. ;
Baltensperger, U. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2011, 116
[10]   Is the gas-particle partitioning in alpha-pinene secondary organic aerosol reversible? [J].
Grieshop, Andrew P. ;
Donahue, Neil M. ;
Robinson, Allen L. .
GEOPHYSICAL RESEARCH LETTERS, 2007, 34 (14)