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DOI | 10.5194/acp-21-1987-2021 |
Measurement report: Sulfuric acid nucleation and experimental conditions in a photolytic flow reactor | |
Hanson D.R.; Menheer S.; Wentzel M.; Kunz J. | |
发表日期 | 2021 |
ISSN | 1680-7316 |
起始页码 | 1987 |
结束页码 | 2001 |
卷号 | 21期号:3 |
英文摘要 | Nucleation rates involving sulfuric acid and water measured in a photolytic flow reactor have decreased considerably over a time period of several years. Results show that the system flow reactor, gas supplies and lines, flow meters, valves, H2SO4 photo-oxidant sources has reached a baseline stability that yields nucleation information such as cluster free energies. The baseline nucleation rate is punctuated by temporary bursts that in many instances are linked to cylinder changes, delineating this source of potential contaminants. Diagnostics were performed to better understand the system, including growth studies to assess H2SO4 levels, chemiluminescent NO and NOx detection to assess the HONO source, and deployment of a second particle detector to assess the nanoparticle detection system. The growth of seed particles shows trends consistent with the sizes of nucleated particles and provides an anchor for calculated H2SO4 concentrations. The chemiluminescent detector revealed that small amounts of NO are present in the HONO source, 10% of HONO. The second condensation-Type particle counter indicates that the nanoparticle mobility sizing system has a bias at low sulfuric acid levels. The measured and modeled nucleation rates represent upper limits to nucleation in the binary homogeneous system, H2SO4-H2O, as contaminants might act to enhance nucleation rates and ion-mediated nucleation may contribute. Nonetheless, the experimental nucleation rates, which have decreased by an order of magnitude or larger since our first publication, extrapolate to some of the lowest rates reported in experiments with photolytic H2SO4. Results from experiments with varying water content and with ammonia addition are also presented and have also decreased by an order of magnitude from our previous work; revised energetics of clusters in this three-component system are derived which differ from our previous energetics mainly in the five-Acid and larger clusters. © 2021 American Society of Mechanical Engineers (ASME). All rights reserved. |
语种 | 英语 |
scopus关键词 | experiment; measurement method; nucleation; photolysis; sulfuric acid; water treatment |
来源期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/247159 |
作者单位 | Chemistry Department, Augsburg University, Minneapolis, MN, United States |
推荐引用方式 GB/T 7714 | Hanson D.R.,Menheer S.,Wentzel M.,et al. Measurement report: Sulfuric acid nucleation and experimental conditions in a photolytic flow reactor[J],2021,21(3). |
APA | Hanson D.R.,Menheer S.,Wentzel M.,&Kunz J..(2021).Measurement report: Sulfuric acid nucleation and experimental conditions in a photolytic flow reactor.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(3). |
MLA | Hanson D.R.,et al."Measurement report: Sulfuric acid nucleation and experimental conditions in a photolytic flow reactor".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.3(2021). |
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