Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer

被引：158

作者：

Chen, Modi ^{[1
]}

Titcombe, Mari ^{[2
,3
]}

Jiang, Jingkun ^{[1
,4
]}

Jen, Coty ^{[1
]}

Kuang, Chongai ^{[5
]}

Fischer, Marc L. ^{[6
]}

Eisele, Fred L. ^{[7
]}

Siepmann, J. Ilja ^{[2
]}

Hanson, David R. ^{[8
]}

Zhao, Jun ^{[1
]}

McMurry, Peter H. ^{[1
]}

机构：

[1] Univ Minnesota, Dept Mech Engn, Minneapolis, MN 55455 USA

[2] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

[3] Colorado Coll, Environm Program, Colorado Springs, CO 80206 USA

[4] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China

[5] Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11973 USA

[6] EO Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Sustainable Energy Syst Grp, Berkeley, CA 94720 USA

[7] Natl Ctr Atmospher Res, Div Atmospher Chem, Boulder, CO 80307 USA

[8] Augsburg Coll, Dept Chem, Minneapolis, MN 55455 USA

来源：

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA | 2012年 / 109卷 / 46期

基金：

美国国家科学基金会;

关键词：

amines; atmospheric aerosol; climate forcing; nanoparticle; chamber study; SULFURIC-ACID; PARTICLE FORMATION; AEROSOL FORMATION; GROWTH-RATES; ATLANTA; EVENTS; H2SO4; WATER;

D O I：

10.1073/pnas.1210285109

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：

Climate models show that particles formed by nucleation can affect cloud cover and, therefore, the earth's radiation budget. Measurements worldwide show that nucleation rates in the atmospheric boundary layer are positively correlated with concentrations of sulfuric acid vapor. However, current nucleation theories do not correctly predict either the observed nucleation rates or their functional dependence on sulfuric acid concentrations. This paper develops an alternative approach for modeling nucleation rates, based on a sequence of acid-base reactions. The model uses empirical estimates of sulfuric acid evaporation rates obtained from new measurements of neutral molecular clusters. The model predicts that nucleation rates equal the sulfuric acid vapor collision rate times a prefactor that is less than unity and that depends on the concentrations of basic gaseous compounds and preexisting particles. Predicted nucleation rates and their dependence on sulfuric acid vapor concentrations are in reasonable agreement with measurements from Mexico City and Atlanta.

引用

页码：18713 / 18718

页数：6

共 40 条

[1]

[Anonymous], CLIM CHANG 2007 IPCC

[2] Laboratory-measured H2SO4-H2O-NH3 ternary homogeneous nucleation rates: Initial observations [J].

Benson, David R. ;

Erupe, Mark E. ;

Lee, Shan-Hu .

GEOPHYSICAL RESEARCH LETTERS, 2009, 36

[3]

Bzdek B. R., 2011, ATMOS CHEM PHYS DISC, V11, P14637, DOI [DOI 10.5194/ACPD-11-14637-2011, 10.5194/acpd-11-14637-2011]

[4] Cluster ion thermal decomposition (I):: Experimental kinetics study and ab initio calculations for HSO4-(H2SO4)x(HNO3)y [J].

Curtius, J ;

Froyd, KD ;

Lovejoy, ER .

JOURNAL OF PHYSICAL CHEMISTRY A, 2001, 105 (48) :10867-10873

[5] Simplified mechanism for new particle formation from methanesulfonic acid, amines, and water via experiments and ab initio calculations [J].

Dawson, Matthew L. ;

Varner, Mychel E. ;

Perraud, Veronique ;

Ezell, Michael J. ;

Gerber, R. Benny ;

Finlayson-Pitts, Barbara J. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (46) :18719-18724

[6] Thermodynamic characterization of Mexico City aerosol during MILAGRO 2006 [J].

Fountoukis, C. ;

Nenes, A. ;

Sullivan, A. ;

Weber, R. ;

Van Reken, T. ;

Fischer, M. ;

Matias, E. ;

Moya, M. ;

Farmer, D. ;

Cohen, R. C. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (06) :2141-2156

[7] Measurement of the thermodynamics of the hydrated dimer and trimer of sulfuric acid [J].

Hanson, D. R. ;

Lovejoy, E. R. .

JOURNAL OF PHYSICAL CHEMISTRY A, 2006, 110 (31) :9525-9528

[8] Measurement of prenucleation molecular clusters in the NH3, H2SO4, H2O system -: art. no. 4158 [J].

Hanson, DR ;

Eisele, FL .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2002, 107 (D12)

[9] Atmospheric ions and nucleation: a review of observations [J].

Hirsikko, A. ;

Nieminen, T. ;

Gagne, S. ;

Lehtipalo, K. ;

Manninen, H. E. ;

Ehn, M. ;

Horrak, U. ;

Kerminen, V-M. ;

Laakso, L. ;

McMurry, P. H. ;

Mirme, A. ;

Mirme, S. ;

Petaja, T. ;

Tammet, H. ;

Vakkari, V. ;

Vana, M. ;

Kulmala, M. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (02) :767-798

[10] Estimating nanoparticle growth rates from size-dependent charged fractions: Analysis of new particle formation events in Mexico City [J].

Iida, Kenjiro ;

Stolzenburg, Mark R. ;

McMurry, Peter H. ;

Smith, James N. .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2008, 113 (D5)

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