Laboratory-measured H2SO4-H2O-NH3 ternary homogeneous nucleation rates: Initial observations

被引:67
作者
Benson, David R. [1 ]
Erupe, Mark E. [1 ]
Lee, Shan-Hu [1 ]
机构
[1] Kent State Univ, Dept Chem, Kent, OH 44420 USA
基金
美国国家科学基金会;
关键词
PARTICLE FORMATION; GAS-PHASE; H2SO4; ACID; H2O; NH3; CLUSTERS;
D O I
10.1029/2009GL038728
中图分类号
P [天文学、地球科学];
学科分类号
07 ;
摘要
We have measured nucleation rates of sulfuric acid-water-ammonia (H2SO4-H2O-NH3) ternary homogeneous nucleation (THN), with a fast flow nucleation reactor attached to two chemical ionization mass spectrometers (CIMSs) to measure H2SO4 and NH3 concentrations simultaneously. Under our experimental conditions with a temperature of 288 K and RH from 4-42% and initial [H2SO4] in the 10(8)-10(9) cm(-3) range and [NH3] from 10-50 ppbv (similar to 2 x 10(11)-1 x 10(12) cm(-3)), the enhancement factor (EF) compared to the binary system ranges up to similar to 1,000 depending on [H2SO4], [NH3] and RH; EF also exponentially increases with decreasing RH and decreasing initial [H2SO4]. The numbers of H2SO4 (9-10) and H2O molecules (6-15) in the critical clusters are reduced in the presence of NH3 [(6-8) and (4-10), respectively]; the number of NH3 molecules in the critical clusters is smaller than 2, under our experimental conditions. Citation: Benson, D. R., M. E. Erupe, and S.-H. Lee (2009), Laboratory-measured H2SO4-H2O-NH3 ternary homogeneous nucleation rates: Initial observations, Geophys. Res. Lett., 36, L15818, doi: 10.1029/2009GL038728.
引用
收藏
页数:6
相关论文
共 30 条
[1]  
[Anonymous], 2006, ATMOS CHEM PHYS
[2]  
Anttila T, 2005, BOREAL ENVIRON RES, V10, P511
[3]   Laboratory studies of particle nucleation:: Initial results for H2SO4, H2O, and NH3 vapors [J].
Ball, SM ;
Hanson, DR ;
Eisele, FL ;
McMurry, PH .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D19) :23709-23718
[4]   The effects of airmass history on new particle formation in the free troposphere: case studies [J].
Benson, D. R. ;
Young, Li-Hao ;
Lee, Shan-Hu ;
Campos, T. L. ;
Rogers, D. C. ;
Jensen, J. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2008, 8 (12) :3015-3024
[5]   Laboratory-measured nucleation rates of sulfuric acid and water binary homogeneous nucleation from the SO2+OHreaction [J].
Benson, David R. ;
Young, Li-Hao ;
Kameel, F. Rifkha ;
Lee, Shan-Hu .
GEOPHYSICAL RESEARCH LETTERS, 2008, 35 (11)
[6]   Rapid formation of sulfuric acid particles at near-atmospheric conditions [J].
Berndt, T ;
Böge, O ;
Stratmann, F ;
Heintzenberg, J ;
Kulmala, M .
SCIENCE, 2005, 307 (5710) :698-700
[7]   MEASUREMENT OF THE GAS-PHASE CONCENTRATION OF H2SO4 AND METHANE SULFONIC-ACID AND ESTIMATES OF H2SO4 PRODUCTION AND LOSS IN THE ATMOSPHERE [J].
EISELE, FL ;
TANNER, DJ .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1993, 98 (D5) :9001-9010
[8]   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
[9]   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)
[10]   Diffusion of H2SO4 in humidified nitrogen:: Hydrated H2SO4 [J].
Hanson, DR ;
Eisele, F .
JOURNAL OF PHYSICAL CHEMISTRY A, 2000, 104 (08) :1715-1719