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Volatility of Mixed Atmospheric Humic-Like Substances and Ammonium Sulfate Particles

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Volatility of Mixed Atmospheric Humic-Like Substances and Ammonium Sulfate Particles CORE Metadata, citation and similar papers at core.ac.uk Provided by Helsingin yliopiston digitaalinen arkisto Atmos. Chem. Phys., 17, 3659–3672, 2017 www.atmos-chem-phys.net/17/3659/2017/ doi:10.5194/acp-17-3659-2017 © Author(s) 2017. CC Attribution 3.0 License. Volatility of mixed atmospheric humic-like substances and ammonium sulfate particles Wei Nie1,2,3,8, Juan Hong3, Silja A. K. Häme3, Aijun Ding1,2,8, Yugen Li4, Chao Yan3, Liqing Hao5, Jyri Mikkilä3, Longfei Zheng1,2,8, Yuning Xie1,2,8, Caijun Zhu1,2,8, Zheng Xu1,2,8, Xuguang Chi1,2,8, Xin Huang1,2,8, Yang Zhou6,7, Peng Lin6,a, Annele Virtanen5, Douglas R. Worsnop3, Markku Kulmala3, Mikael Ehn3, Jianzhen Yu6, Veli-Matti Kerminen3, and Tuukka Petäjä3,1 1Joint International Research Laboratory of Atmospheric and Earth System Sciences, Nanjing University, Nanjing, China 2Institute for Climate and Global Change Research & School of Atmospheric Sciences, Nanjing University, Nanjing, 210023, China 3Division of Atmospheric Sciences, Department of Physics, University of Helsinki, Helsinki, Finland 4Division of Environment, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong SAR, China 5Department of Applied Physics, University of Eastern Finland, Kuopio 70211, Finland 6Department of Chemistry, Hong Kong University of Science & Technology, Clear Water Bay, Kowloon, Hong Kong SAR, China 7Key Laboratory of Physical Oceanography, College of Oceanic and Atmospheric Sciences, Ocean University of China, Qingdao 266100, China 8Collaborative Innovation Center of Climate Change, Jiangsu province, China anow at: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99532, USA Correspondence to: Wei Nie ([email protected]) and Aijun Ding ([email protected]) Received: 20 September 2016 – Discussion started: 11 October 2016 Revised: 27 February 2017 – Accepted: 28 February 2017 – Published: 15 March 2017 Abstract. The volatility of organic aerosols remains poorly semi-volatile (SVOC), low-volatility (LVOC) and extremely understood due to the complexity of speciation and multi- low-volatility components (ELVOC). The results showed that phase processes. In this study, we extracted humic-like sub- LVOC and ELVOC dominated (more than 80 %) the total vol- stances (HULIS) from four atmospheric aerosol samples col- ume of HULIS. Atomizing processes led to a size-dependent lected at the SORPES station in Nanjing, eastern China, evaporation of regenerated HULIS particles, and resulted in and investigated the volatility behavior of particles at dif- more ELVOC in smaller particles. In order to understand the ferent sizes using a Volatility Tandem Differential Mobil- role of interaction between inorganic salts and atmospheric ity Analyzer (VTDMA). In spite of the large differences organic mixtures in the volatility of an organic aerosol, the in particle mass concentrations, the extracted HULIS from evaporation of mixed samples of ammonium sulfate (AS) the four samples all revealed very high-oxidation states and HULIS was measured. The results showed a significant (O : C > 0.95), indicating secondary formation as the major but nonlinear influence of ammonium sulfate on the volatil- source of HULIS in Yangtze River Delta (YRD). An overall ity of HULIS. The estimated fraction of ELVOC in the or- low volatility was identified for the extracted HULIS, with ganic part of the largest particles (145 nm) increased from the volume fraction remaining (VFR) higher than 55 % for 26 %, in pure HULIS samples, to 93 % in 1 : 3 (mass ratio of all the regenerated HULIS particles at the temperature of HULIS : AS) mixed samples, to 45 % in 2 : 2 mixed samples, 280 ◦C. A kinetic mass transfer model was applied to the and to 70 % in 3 : 1 mixed samples, suggesting that the inter- thermodenuder (TD) data to interpret the observed evapora- action with ammonium sulfate tends to decrease the volatility tion pattern of HULIS, and to derive the mass fractions of of atmospheric organic compounds. Our results demonstrate Published by Copernicus Publications on behalf of the European Geosciences Union. 3660 W. Nie et al.: Volatility of mixed atmospheric humic-like substances and ammonium sulfate particles that HULIS are important low-volatility, or even extremely ganic and several inorganic compounds. One way to interlink low-volatility, compounds in the organic-aerosol phase. As laboratory and ambient studies, and to understand the volatil- important formation pathways of atmospheric HULIS, multi- ity of ambient OA systematically, might be to isolate some phase processes, including oxidation, oligomerization, poly- classes of OA from ambient particles before investigating merization and interaction with inorganic salts, are indicated their volatility separately. As an important subgroup of or- to be important sources of low-volatility and extremely low- ganic aerosols in the real ambient aerosols, the physicochem- volatility species of organic aerosols. ical properties of HULIS have been studied widely, including their mass concentrations (Lin et al., 2010b), chemical com- position (Lin et al., 2012; Kristensen et al., 2015; Chen et al., 2016), density (Dinar et al., 2006), and hygroscopicity (Wex 1 Introduction et al., 2007; Kristensen et al., 2014). However, to the best of our knowledge, the volatility of atmospheric HULIS has Atmospheric organic aerosol (OA) comprises 20–90 % of never been reported so far. the total submicron aerosol mass, depending on location In the ambient aerosol, organic aerosol (OA, including (Kanakidou et al., 2005; Zhang et al., 2007; Jimenez et al., HULIS) mostly co-exist with inorganic compounds, such as 2009), and plays a critical role in air quality and global ammonium sulfate. The volatility of OA has been demon- climate change. Given the large variety of organic species, strated to be affected by aerosol-phase reactions when mixed OA is typically grouped in different ways according to its with inorganic compounds (Bilde et al., 2015). The most typ- sources and physicochemical properties. These include the ical examples of these are interactions between particulate in- classifications based on aerosol optical properties (brown organic salts with organic acids to form organic salts, which carbon and non-light-absorbing OA), formation pathways evidently can enhance the partitioning of organic acids onto (primary (POA) and secondary (SOA) organic aerosol), and the aerosol phase (Zardini et al., 2010; Laskin et al., 2012; solubility (water-soluble OA (WSOA) and water-insoluble Häkkinen et al., 2014; Yli-Juuti et al., 2013). Recent stud- OA (WISOA)). Humic-like substances (HULIS), according ies have reported that the saturation vapor pressure (psat/ of to their operational definition, are the hydrophobic part of ammonium oxalate is significantly lower than that of pure −6 WSOA, and contribute to more than half of the WSOA oxalic acid, with psat being around 10 Pa for ammonium (e.g., Krivácsy et al., 2008). Secondary formation (Lin et al., oxalate (Ortiz-Montalvo et al., 2014; Paciga et al., 2014). 2010b) and primary emission from biomass burning (Lukács However, this has not shown to be the case for adipic acid et al., 2007; Lin et al., 2010a) have been identified as the vs. ammonium adipate, indicating that not all dicarboxylic two major sources of atmospheric HULIS. Because they acids react with ammonium to form low-volatility organic are abundantly present, water-soluble, light-absorbing and salts (Paciga et al., 2014). Given that HULIS contain acidic surface-active, HULIS in atmospheric particles have been species (Paglione et al., 2014; Chen et al., 2016), their in- demonstrated to play important roles in several processes, teraction with inorganic salts would plausibly influence their including cloud droplet formation, light absorption and het- volatility. erogeneous redox activities (Kiss et al., 2005; Graber and In this study, HULIS were extracted from PM2:5 filter sam- Rudich, 2006; Hoffer et al., 2006; Lukács et al., 2007; Lin ples collected at the SORPES station (Station for observing and Yu, 2011; Verma et al., 2012; Kristensen et al., 2012). Regional Processes of the Earth System) in western Yangtze Volatility of atmospheric organic compounds is one of River Delta (YRD) during the winter of 2014 to 2015. A their key physical properties determining their partitioning Volatility-Hygroscopicity Tandem Differential Mobility An- between the gas and aerosol phases, thereby strongly in- alyzer (VH-TDMA) was then used to measure the volatil- fluencing their lifetimes and concentrations. Atmospheric ity properties of extracted HULIS and their mixtures with OA can be divided into semi-volatile organic compounds ammonium sulfate. A kinetic mass transfer model was de- (SVOC), low-volatility organic compounds (LVOC) and ex- ployed to rebuild the measured thermograms, and to sep- tremely low-volatility organic compounds (ELVOC) (Don- arate the mixture into three volatility fractions having an ahue et al., 2012; Murphy et al., 2014). LVOC and ELVOC extremely low volatility, low volatility and semi-volatility. are predominantly in the aerosol phase and contribute largely Our main goals were (1) to characterize the volatility of to the new particle formation and growth (Ehn et al., 2014), size-dependent, regenerated HULIS particles and to get in- while SVOC have considerable mass fractions in both phases sight into the relationship between atmospheric HULIS and and usually dominate the mass concentration of OA. As far ELVOC, and (2) to
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