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DOI | 10.5194/acp-19-8999-2019 |
H2SO4 and particle production in a photolytic flow reactor: chemical modeling, cluster thermodynamics and contamination issues | |
Hanson, David R.1; Abdullahi, Hussein1; Menheer, Seakh1; Vences, Joaquin1; Alves, Michael R.1,2; Kunz, Joan1 | |
2019-07-17 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2019 |
卷号 | 19期号:14页码:8999-9015 |
文章类型 | Article |
语种 | 英语 |
国家 | USA |
英文摘要 | Size distributions of particles formed from sulfuric acid (H2SO4) and water vapor in a photolytic flow reactor (PhoFR) were measured with a nanoparticle mobility sizing system. Experiments with added ammonia and dimethylamine were also performed. H2SO4(g) was synthesized from HONO, sulfur dioxide and water vapor, initiating OH oxidation by HONO photolysis. Experiments were performed at 296K over a range of sulfuric acid production levels and for 16% to 82% relative humidity. Measured distributions generally had a large-particle mode that was roughly lognormal; mean diameters ranged from 3 to 12 nm and widths (ln sigma) were similar to 0.3. Particle formation conditions were stable over many months. Addition of single-digit pmol mol 1 mixing ratios of dimethylamine led to very large increases in particle number density. Particles produced with ammonia, even at 2000 pmol mol(-1), showed that NH3 is a much less effective nucleator than dimethylamine. A two-dimensional simulation of particle formation in PhoFR is also presented that starts with gas-phase photolytic production of H2SO4, followed by kinetic formation of molecular clusters and their decomposition, which is determined by their thermodynamics. Comparisons with model predictions of the experimental result's dependency on HONO and water vapor concentrations yield phenomenological cluster thermodynamics and help delineate the effects of potential contaminants. The added-base simulations and experimental results provide support for previously published dimethylamine-H2SO4 cluster thermodynamics and provide a phenomenological set of ammonia-sulfuric acid thermodynamics. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000475760800001 |
WOS关键词 | COMPUTATIONAL FLUID-DYNAMICS ; SULFURIC-ACID-WATER ; GROWTH-RATES ; HOMOGENEOUS NUCLEATION ; OXIDATION-PRODUCTS ; FREE-ENERGIES ; SO2 ; HO2 ; AMMONIA ; AEROSOL |
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/185157 |
专题 | 地球科学 |
作者单位 | 1.Augsburg Univ, Chem Dept, Minneapolis, MN 55454 USA; 2.Univ Calif San Diego, Chem & Biochem, La Jolla, CA 92093 USA |
推荐引用方式 GB/T 7714 | Hanson, David R.,Abdullahi, Hussein,Menheer, Seakh,et al. H2SO4 and particle production in a photolytic flow reactor: chemical modeling, cluster thermodynamics and contamination issues[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(14):8999-9015. |
APA | Hanson, David R.,Abdullahi, Hussein,Menheer, Seakh,Vences, Joaquin,Alves, Michael R.,&Kunz, Joan.(2019).H2SO4 and particle production in a photolytic flow reactor: chemical modeling, cluster thermodynamics and contamination issues.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(14),8999-9015. |
MLA | Hanson, David R.,et al."H2SO4 and particle production in a photolytic flow reactor: chemical modeling, cluster thermodynamics and contamination issues".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.14(2019):8999-9015. |
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