气候变化领域集成服务门户(CCPortal): H2SO4 and particle production in a photolytic flow reactor: Chemical modeling; cluster thermodynamics and contamination issues

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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 D.; Abdullahi H.; Menheer S.; Vences J.; Alves M.; Kunz J.
发表日期	2019
ISSN	16807316
起始页码	8999
结束页码	9015
卷号	19 期号:14
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 296 K 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 (lnσ) were ĝ1/40.3. 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. © 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
语种	英语
scopus关键词	bioreactor; hydrogen sulfide; particle size; particulate matter; photolysis; pollutant; size distribution; sulfuric acid; thermodynamics; water vapor
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/144278
作者单位	Chemistry Department, Augsburg University, Minneapolis, MN 55454, United States; Chemistry and Biochemistry, University of California, San Diego, CA 92093, United States
推荐引用方式 GB/T 7714	Hanson D.,Abdullahi H.,Menheer S.,et al. H2SO4 and particle production in a photolytic flow reactor: Chemical modeling; cluster thermodynamics and contamination issues[J],2019,19(14).
APA	Hanson D.,Abdullahi H.,Menheer S.,Vences J.,Alves M.,&Kunz J..(2019).H2SO4 and particle production in a photolytic flow reactor: Chemical modeling; cluster thermodynamics and contamination issues.Atmospheric Chemistry and Physics,19(14).
MLA	Hanson D.,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).