How salt lakes affect atmospheric new particle formation: A case study in Western Australia

Kamilli, Katharina; Ofner, Johannes; Krause, Torsten; Sattler, Tobias; Schmitt‐Kopplin, Philippe; Eitenberger, Elisabeth; Friedbacher, Gernot; Lendl, Bernhard; Lohninger, Hans; Schöler, H. F.; Held, Andreas

doi:10.1016/j.scitotenv.2016.08.058

Cited by 8 publications

(10 citation statements)

References 37 publications

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“…The uptake of HCl produced from hydrogen abstraction or intramolecular HCl elimination could also contribute slightly to observed particulate chlorine. Organochloride has also been observed in biogenic SOA post-processed by halogenation (Ofner et al, 2012), in new particles formed from 1,8-cineol and limonene over simulated salt lakes (Kamilli et al, 2015), and in situ over salt lakes (Kamilli et al, 2016). To date, this is the only reported study of organochloride measurement using an ACSM.…”

Section: Particulate Organochloridementioning

confidence: 85%

“…Reactive halogen species in the form of X 2 , XO, HOX, XNO 2 , and OXO are present in polar regions (Buys et al, 2013;Liao et al, 2014;Pöhler et al, 2010), the MBL (Lawler et al, 2011;Read et al, 2008), and coastal and inland regions (Mielke et al, 2013;Riedel et al, 2012Riedel et al, , 2013. Outside of the MBL and polar regions, natural emissions of reactive halogen species have been observed in volcano plumes (Bobrowski et al, 2007) and over salt lakes (Kamilli et al, 2016;Stutz, 2002). Anthropogenic sources include industrial emissions (Chang and Allen, 2006;Riedel et al, 2013;Tanaka et al, 2003), oil and gas production , water treatment (Chang et al, 2001), biomass burning (Lobert et al, 1999), engine exhaust (Osthoff et al, 2008;Parrish et al, 2009), and NO x -mediated heterogenous reactions, notably the production of ClNO 2 via reactive uptake of N 2 O 5 onto particles containing Cl − (Thornton et al, 2010).…”

Section: S Wang and L Hildebrandt Ruiz: Secondary Organic Aerosomentioning

confidence: 99%

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Secondary organic aerosol from chlorine-initiated oxidation of isoprene

Wang

Ruiz

2017

Atmos. Chem. Phys.

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Abstract. Recent studies have found concentrations of reactive chlorine species to be higher than expected, suggesting that atmospheric chlorine chemistry is more extensive than previously thought. Chlorine radicals can interact with hydroperoxy (HO x ) radicals and nitrogen oxides (NO x ) to alter the oxidative capacity of the atmosphere. They are known to rapidly oxidize a wide range of volatile organic compounds (VOCs) found in the atmosphere, yet little is known about secondary organic aerosol (SOA) formation from chlorineinitiated photooxidation and its atmospheric implications. Environmental chamber experiments were carried out under low-NO x conditions with isoprene and chlorine as primary VOC and oxidant sources. Upon complete isoprene consumption, observed SOA yields ranged from 7 to 36 %, decreasing with extended photooxidation and SOA aging. Formation of particulate organochloride was observed. A highresolution time-of-flight chemical ionization mass spectrometer was used to determine the molecular composition of gasphase species using iodide-water and hydronium-water cluster ionization. Multi-generational chemistry was observed, including ions consistent with hydroperoxides, chloroalkyl hydroperoxides, isoprene-derived epoxydiol (IEPOX), and hypochlorous acid (HOCl), evident of secondary OH production and resulting chemistry from Cl-initiated reactions. This is the first reported study of SOA formation from chlorineinitiated oxidation of isoprene. Results suggest that tropospheric chlorine chemistry could contribute significantly to organic aerosol loading.

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Section: Particulate Organochloridementioning

confidence: 85%

Section: S Wang and L Hildebrandt Ruiz: Secondary Organic Aerosomentioning

confidence: 99%

Secondary organic aerosol from chlorine-initiated oxidation of isoprene

Wang

Ruiz

2017

Atmos. Chem. Phys.

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“…The salt lakes of the Australian wheat belt have been identified to be a source of ultrafine particles which were measured in elevated numbers over the agricultural land by airborne, car-based and stationary instruments [53,54]. This raised the question of the underlying aerosol formation process and whether the salt lakes have a significant impact on the local climate that unambiguously changed over the last decades.…”

Section: Discussionmentioning

confidence: 99%

“…The pH was measured to be around 7.3 (see Table 1 for an overview of lake characteristics). Sampling locations were selected in the context of SOA formation events [53,54] and to cover a broad range of geochemical characteristics. For a detailed site description refer to Krause [9].…”

Section: Methodsmentioning

confidence: 99%

Natural Formation of Chloro- and Bromoacetone in Salt Lakes of Western Australia

et al. 2019

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Western Australia is a semi-/arid region known for saline lakes with a wide range of geochemical parameters (pH 2.5-7.1, Cl − 10-200 g L −1 ). This study reports on the haloacetones chloroand bromoacetone in air over 6 salt lake shorelines. Significant emissions of chloroacetone (up to 0.2 µmol m −2 h −1 ) and bromoacetone (up to 1. 5 µmol m −2 h −1 ) were detected, and a photochemical box model was employed to evaluate the contribution of their atmospheric formation from the olefinic hydrocarbons propene and methacrolein in the gas phase. The measured concentrations could not explain the photochemical halogenation reaction, indicating a strong hitherto unknown source of haloacetones. Aqueous-phase reactions of haloacetones, investigated in the laboratory using humic acid in concentrated salt solutions, were identified as alternative formation pathway by liquid-phase reactions, acid catalyzed enolization of ketones, and subsequent halogenation. In order to verify this mechanism, we made measurements of the Henry's law constants, rate constants for hydrolysis and nucleophilic exchange with chloride, UV-spectra and quantum yields for the photolysis of bromoacetone and 1,1-dibromoacetone in the aqueous phase. We suggest that heterogeneous processes induced by humic substances in the quasi-liquid layer of the salt crust, particle surfaces and the lake water are the predominating pathways for the formation of the observed haloacetones.

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“…Short-term exposure to aerosol could also induce stress response and cytotoxicity in cells (de Bruijne et al, 2009;Ebersviller et al, 2012;Hawley et al, 2014). Equilibrium partitioning of oxidized, semi-volatile organic compounds (Pankow, 1994), collectively referred to as secondary organic aerosol (SOA), contributes 20-90 % of the global fine aerosol budget (Jimenez et al, 2009;Kanakidou et al, 2005). The majority of SOA originates from oxidation of biogenic volatile organic compounds (BVOCs), which account for ∼ 90% of annual non-methane hydrocarbon emissions (Goldstein and Galbally, 2007;Guenther et al, 2012), among which isoprene has the highest emission rate at ∼ 600 Tg yr −1 (Guenther et al, 2006).…”

Section: Introductionmentioning

confidence: 99%

Secondary organic aerosol from chlorine-initiated oxidation of isoprene

Wang¹,

Ruiz²

2017

Preprint

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Abstract. Recent studies have found inland concentrations of reactive chlorine species to be higher than expected, suggesting that atmospheric chlorine chemistry is more extensive than previously thought. Chlorine radicals can interact with HOx radicals and nitrogen oxides (NOx) to alter the oxidative capacity of the atmosphere. They are known to rapidly oxidize a wide range of volatile organic compounds (VOC) found in the atmosphere, yet little is known about secondary organic aerosol (SOA) formation from chlorine-initiated photo-oxidation and its atmospheric implications. Environmental chamber experiments were carried out under low-NOx conditions with isoprene and chlorine as primary VOC and oxidant sources. Upon complete isoprene consumption, observed SOA yields ranged from 8&#8201;% to 36&#8201;%, decreasing with extended photo-oxidation and SOA aging. A High-Resolution Time-of-Flight Chemical Ionization Mass Spectrometer was used to determine the molecular composition of gas-phase species using iodide-water and hydronium-water ionization. Ions consistent with isoprene-derived epoxydiol (IEPOX) and other common OH-isoprene oxidation products were observed, evident of secondary OH production and resulting chemistry from Cl-initiated reactions.

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How salt lakes affect atmospheric new particle formation: A case study in Western Australia

Cited by 8 publications

References 37 publications

Secondary organic aerosol from chlorine-initiated oxidation of isoprene

Secondary organic aerosol from chlorine-initiated oxidation of isoprene

Natural Formation of Chloro- and Bromoacetone in Salt Lakes of Western Australia

Secondary organic aerosol from chlorine-initiated oxidation of isoprene

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