ALPHA-PINENE;
CHEMICAL-COMPOSITION;
HETEROGENEOUS REACTIONS;
ALPHA-PINENE/O-3;
REACTION;
TERPENE OZONOLYSIS;
PARTICULATE MATTER;
EMISSION INVENTORY;
ABSORPTION-MODEL;
TRANSPORT MODEL;
GLOBAL AEROSOL;
D O I:
10.5194/acp-9-7003-2009
中图分类号:
X [环境科学、安全科学];
学科分类号:
08 ;
0830 ;
摘要:
The role of isoprene as a precursor to secondary organic aerosol (SOA) over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr(-1) and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of organic matter ( OM) during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC) emissions from vegetation. However, during winter, our model strongly underestimates OM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning) of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr(-1)). The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights in isoprene SOA formation mechanisms reduces the tropospheric production of isoprene derived SOA over Europe from 0.4 Tg yr(-1) in our reference simulation to 0.1 Tg yr(-1).
机构:
US EPA, Off Res & Dev, Atmospher Modeling & Anal Div, Res Triangle Pk, NC 27711 USAUS EPA, Off Res & Dev, Atmospher Modeling & Anal Div, Res Triangle Pk, NC 27711 USA
Carlton, A. G.
Wiedinmyer, C.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Natl Ctr Atmospher Res, Div Atmospher Chem, Boulder, CO 80309 USAUS EPA, Off Res & Dev, Atmospher Modeling & Anal Div, Res Triangle Pk, NC 27711 USA
Wiedinmyer, C.
Kroll, J. H.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res Inc, Billerica, MA 01821 USAUS EPA, Off Res & Dev, Atmospher Modeling & Anal Div, Res Triangle Pk, NC 27711 USA
机构:
CIRES, Boulder, CO 80309 USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USACIRES, Boulder, CO 80309 USA
Krechmer, Jordan E.
Coggon, Matthew M.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USACIRES, Boulder, CO 80309 USA
Coggon, Matthew M.
Massoli, Paola
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USACIRES, Boulder, CO 80309 USA
Massoli, Paola
Nguyen, Tran B.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USACIRES, Boulder, CO 80309 USA
Nguyen, Tran B.
Crounse, John D.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USACIRES, Boulder, CO 80309 USA
Crounse, John D.
Hu, Weiwei
论文数: 0|引用数: 0|
h-index: 0|
机构:
CIRES, Boulder, CO 80309 USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USACIRES, Boulder, CO 80309 USA
Hu, Weiwei
Day, Douglas A.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USACIRES, Boulder, CO 80309 USA
Day, Douglas A.
Tyndall, Geoffrey S.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USA
Natl Ctr Atmospher Res, Boulder, CO USACIRES, Boulder, CO 80309 USA
Tyndall, Geoffrey S.
Henze, Daven K.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Univ Colorado, Dept Engn Mech, Boulder, CO 80309 USACIRES, Boulder, CO 80309 USA
Henze, Daven K.
Rivera-Rios, Jean C.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Univ Wisconsin, Dept Chem, Madison, WI 53706 USACIRES, Boulder, CO 80309 USA
Rivera-Rios, Jean C.
Nowak, John B.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USACIRES, Boulder, CO 80309 USA
Nowak, John B.
Kimmel, Joel R.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USA
Tofwerk AG, CH-3600 Thun, SwitzerlandCIRES, Boulder, CO 80309 USA
Kimmel, Joel R.
Mauldin, Roy L., III
论文数: 0|引用数: 0|
h-index: 0|
机构:
Univ Colorado, Dept Atmospher & Ocean Sci, Boulder, CO 80309 USACIRES, Boulder, CO 80309 USA
Mauldin, Roy L., III
Stark, Harald
论文数: 0|引用数: 0|
h-index: 0|
机构:
CIRES, Boulder, CO 80309 USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USACIRES, Boulder, CO 80309 USA
Stark, Harald
Jayne, John T.
论文数: 0|引用数: 0|
h-index: 0|
机构:CIRES, Boulder, CO 80309 USA
Jayne, John T.
Sipila, Mikko
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USA
Univ Helsinki, Dept Phys, FIN-00014 Helsinki, FinlandCIRES, Boulder, CO 80309 USA
Sipila, Mikko
Junninen, Heikki
论文数: 0|引用数: 0|
h-index: 0|
机构:
Univ Helsinki, Dept Phys, FIN-00014 Helsinki, FinlandCIRES, Boulder, CO 80309 USA
Junninen, Heikki
St. Clair, Jason M.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USACIRES, Boulder, CO 80309 USA
St. Clair, Jason M.
Zhang, Xuan
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USACIRES, Boulder, CO 80309 USA
Zhang, Xuan
Feiner, Philip A.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Penn State Univ, Dept Meteorol, University Pk, PA 16802 USACIRES, Boulder, CO 80309 USA
Feiner, Philip A.
Zhang, Li
论文数: 0|引用数: 0|
h-index: 0|
机构:
Penn State Univ, Dept Meteorol, University Pk, PA 16802 USACIRES, Boulder, CO 80309 USA
Zhang, Li
Miller, David O.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Penn State Univ, Dept Meteorol, University Pk, PA 16802 USACIRES, Boulder, CO 80309 USA
Miller, David O.
Brune, William H.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Penn State Univ, Dept Meteorol, University Pk, PA 16802 USACIRES, Boulder, CO 80309 USA
Brune, William H.
Keutsch, Frank N.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Univ Wisconsin, Dept Chem, Madison, WI 53706 USACIRES, Boulder, CO 80309 USA
Keutsch, Frank N.
Wennberg, Paul O.
论文数: 0|引用数: 0|
h-index: 0|
机构:CIRES, Boulder, CO 80309 USA
Wennberg, Paul O.
Seinfeld, John H.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USACIRES, Boulder, CO 80309 USA
Seinfeld, John H.
Worsnop, Douglas R.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USACIRES, Boulder, CO 80309 USA
Worsnop, Douglas R.
Jimenez, Jose L.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CIRES, Boulder, CO 80309 USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USACIRES, Boulder, CO 80309 USA
Jimenez, Jose L.
Canagaratna, Manjula R.
论文数: 0|引用数: 0|
h-index: 0|
机构:
Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USACIRES, Boulder, CO 80309 USA
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Surratt, Jason D.
Chan, Arthur W. H.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Chan, Arthur W. H.
Eddingsaas, Nathan C.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Eddingsaas, Nathan C.
Chan, ManNin
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Chan, ManNin
Loza, Christine L.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Loza, Christine L.
Kwan, Alan J.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Kwan, Alan J.
Hersey, Scott P.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Hersey, Scott P.
Flagan, Richard C.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Flagan, Richard C.
Wennberg, Paul O.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA
CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
Wennberg, Paul O.
Seinfeld, John H.
论文数: 0|引用数: 0|
h-index: 0|
机构:
CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USACALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA