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Influence of seed aerosol surface area and oxidation rate on vapor wall deposition and SOA mass yields: a case study with α-pinene ozonolysis
被引:66
作者:
Nah, Theodora
[1
]
Mcvay, Renee C.
[2
]
Zhang, Xuan
[3
,5
]
Boyd, Christopher M.
[1
]
Seinfeld, John H.
[2
,3
]
Ng, Nga L.
[1
,4
]
机构:
[1] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[2] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
[3] CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA
[4] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[5] Aerodyne Res, Ctr Aerosol & Cloud Chem, Billerica, MA USA
基金:
美国国家科学基金会;
关键词:
SECONDARY ORGANIC AEROSOL;
BIOGENIC HYDROCARBONS;
PARTICLE-PHASE;
M-XYLENE;
SEMIVOLATILE ORGANICS;
LABORATORY CHAMBERS;
NO3;
OXIDATION;
SMOG-CHAMBER;
GAS;
VOLATILITY;
D O I:
10.5194/acp-16-9361-2016
中图分类号:
X [环境科学、安全科学];
学科分类号:
08 ;
0830 ;
摘要:
Laboratory chambers, invaluable in atmospheric chemistry and aerosol formation studies, are subject to particle and vapor wall deposition, processes that need to be accounted for in order to accurately determine secondary organic aerosol (SOA) mass yields. Although particle wall deposition is reasonably well understood and usually accounted for, vapor wall deposition is less so. The effects of vapor wall deposition on SOA mass yields in chamber experiments can be constrained experimentally by increasing the seed aerosol surface area to promote the preferential condensation of SOA-forming vapors onto seed aerosol. Here, we study the influence of seed aerosol surface area and oxidation rate on SOA formation in alpha-pinene ozonolysis. The observations are analyzed using a coupled vapor-particle dynamics model to interpret the roles of gas-particle partitioning (quasi-equilibrium vs. kinetically limited SOA growth) and alpha-pinene oxidation rate in influencing vapor wall deposition. We find that the SOA growth rate and mass yields are independent of seed surface area within the range of seed surface area concentrations used in this study. This behavior arises when the condensation of SOA-forming vapors is dominated by quasi-equilibrium growth. Faster alpha-pinene oxidation rates and higher SOA mass yields are observed at increasing O-3 concentrations for the same initial alpha-pinene concentration. When the alpha-pinene oxidation rate increases relative to vapor wall deposition, rapidly produced SOA-forming oxidation products condense more readily onto seed aerosol particles, resulting in higher SOA mass yields. Our results indicate that the extent to which vapor wall deposition affects SOA mass yields depends on the particular volatility organic compound system and can be mitigated through the use of excess oxidant concentrations.
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页码:9361 / 9379
页数:19
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