Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-18-12433-2018 |
Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling | |
Hodshire, Anna L.1; Palm, Brett B.2,3,14; Alexander, M. Lizabeth4; Bian, Qijing1; Campuzano-Jost, Pedro2,3; Cross, Eben S.5,15; Day, Douglas A.2,3; de Sa, Suzane S.6; Guenther, Alex B.7,8; Hansel, Armin9; Hunter, James F.5; Jud, Werner9,16; Karl, Thomas10; Kim, Saewung7; Kroll, Jesse H.4,11; Park, Jeong-Hoo12,17; Peng, Zhe2,3; Seco, Roger7; Smith, James N.13; Jimenez, Jose L.2,3; Pierce, Jeffrey R.1 | |
2018-08-28 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:16页码:12433-12460 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Austria; Germany; South Korea |
英文摘要 | Oxidation flow reactors (OFRs) allow the concentration of a given atmospheric oxidant to be increased beyond ambient levels in order to study secondary organic aerosol (SOA) formation and aging over varying periods of equivalent aging by that oxidant. Previous studies have used these reactors to determine the bulk OA mass and chemical evolution. To our knowledge, no OFR study has focused on the interpretation of the evolving aerosol size distributions. In this study, we use size-distribution measurements of the OFR and an aerosol microphysics model to learn about size-dependent processes in the OFR. Specifically, we use OFR exposures between 0.09 and 0.9 equivalent days of OH aging from the 2011 BEACHON-RoMBAS and GoAmazon2014/5 field campaigns. We use simulations in the TOMAS (TwO-Moment Aerosol Sectional) microphysics box model to constrain the following parameters in the OFR: (1) the rate constant of gas-phase functionalization reactions of organic compounds with OH, (2) the rate constant of gas-phase fragmentation reactions of organic compounds with OH, (3) the reactive uptake coefficient for heterogeneous fragmentation reactions with OH, (4) the nucleation rate constants for three different nucleation schemes, and (5) an effective accommodation coefficient that accounts for possible particle diffusion limitations of particles larger than 60 nm in diameter. We find the best model-to-measurement agreement when the accommodation coefficient of the larger particles (D-p > 60 nm) was 0.1 or lower (with an accommodation co-efficient of 1 for smaller particles), which suggests a diffusion limitation in the larger particles. When using these low accommodation-coefficient values, the model agrees with measurements when using a published H2SO4-organics nucleation mechanism and previously published values of rate constants for gas-phase oxidation reactions. Further, gas-phase fragmentation was found to have a significant impact upon the size distribution, and including fragmentation was necessary for accurately simulating the distributions in the OFR. The model was insensitive to the value of the reactive uptake coefficient on these aging timescales. Monoterpenes and isoprene could explain 24%-95% of the observed change in total volume of aerosol in the OFR, with ambient semivolatile and intermediate-volatility organic compounds (S/IVOCs) appearing to explain the remainder of the change in total volume. These results provide support to the mass-based findings of previous OFR studies, give insight to important size-distribution dynamics in the OFR, and enable the design of future OFR studies focused on new particle formation and/or microphysical processes. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000442942600002 |
WOS关键词 | SECONDARY ORGANIC AEROSOL ; HETEROGENEOUS OH OXIDATION ; ATMOSPHERIC SULFURIC-ACID ; LOW-VOLATILITY SOA ; PARTICLE FORMATION ; TEMPERATURE-DEPENDENCE ; PARTICULATE MATTER ; FRAGMENTATION REACTIONS ; CHEMICAL-COMPOSITION ; RADICAL CHEMISTRY |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/27251 |
专题 | 地球科学 |
作者单位 | 1.Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA; 2.Univ Colorado, Dept Chem, Boulder, CO 80309 USA; 3.Univ Colorado, CIRES, Boulder, CO 80309 USA; 4.Pacific Northwest Natl Lab, Environm & Mol Sci Lab, Richland, WA 99352 USA; 5.MIT, Dept Civil & Environm Engn, 77 Massachusetts Ave, Cambridge, MA 02139 USA; 6.Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA; 7.Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA 92697 USA; 8.Pacific Northwest Natl Lab, Div Atmospher Sci & Global Change, Richland, WA 99352 USA; 9.Univ Innsbruck, Inst Ion & Appl Phys, A-6020 Innsbruck, Austria; 10.Univ Innsbruck, Inst Atmospher & Cryospher Sci, A-6020 Innsbruck, Austria; 11.MIT, Dept Chem Engn, Cambridge, MA 02139 USA; 12.Natl Ctr Atmospher Res, Boulder, CO 80305 USA; 13.Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA; 14.Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA; 15.Aerodyne Res Inc, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USA; 16.Helmholtz Zentrum Munchen, Res Unit Environm Simulat, Inst Biochem Plant Pathol, D-85764 Munich, Germany; 17.Natl Inst Environm Res, Climate & Air Qual Res Dept, Incheon 22689, South Korea |
推荐引用方式 GB/T 7714 | Hodshire, Anna L.,Palm, Brett B.,Alexander, M. Lizabeth,et al. Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(16):12433-12460. |
APA | Hodshire, Anna L..,Palm, Brett B..,Alexander, M. Lizabeth.,Bian, Qijing.,Campuzano-Jost, Pedro.,...&Pierce, Jeffrey R..(2018).Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(16),12433-12460. |
MLA | Hodshire, Anna L.,et al."Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.16(2018):12433-12460. |
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