Increasing Isoprene Epoxydiol-to-Inorganic Sulfate Aerosol Ratio Results in Extensive Conversion of Inorganic Sulfate to Organosulfur Forms: Implications for Aerosol Physicochemical Properties

Riva, Matthieu; Chen, Yuzhi; Zhang, Yue; Lei, Ziying; Olson, Nicole E.; Boyer, Hallie C.; Narayan, Shweta; Yee, L. D.; Green, Hilary S.; Cui, Tianqu; Zhang, Zhenfa; Baumann, Karsten; Fort, Mike; Edgerton, Eric S.; Budisulistiorini, Sri Hapsari; Rose, C. A.; Ribeiro, Igor O.; Oliveira, Rafael Lopes; Santos, Erickson Oliveira dos; Machado, Cristine M. D.; Szopa, Sophie; Zhao, Yue; Alves, Eliane Gomes; Sá, Suzane S. de; Hu, Weiwei; Knipping, Eladio; Shaw, Stephanie L.; Duvoisin, Sérgio; Souza, Rodrigo Augusto Ferreira de; Palm, Brett B.; Jimenez, José L.; Glasius, Marianne; Goldstein, Allen H.; Pye, Havala O. T.; Gold, Avram; Turpin, Barbara J.; Vizuete, William; Martin, Scot T.; Thornton, Joel A.; Dutcher, Cari S.; Ault, Andrew P.; Surratt, Jason D.

doi:10.1021/acs.est.9b01019

Cited by 137 publications

(307 citation statements)

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“…These are inaccessible experimentally because electrolyte solutions (of any relevant amount of substance) always contain both cations and anions, in proportions yielding an overall electroneutral system. Only mean activity coefficients of neutral cation-anion combinations are measurable quantities, such as γ ±,HCl = γ H + γ Cl − 1 2 in the case of the 1 : 1 electrolyte HCl (e.g., Prausnitz et al, 1999;Robinson and Stokes, 2002). Several, but not all, thermodynamic activity coefficient models used in atmospheric science and geochemistry provide a computation of single-ion activity coefficients within their mathematical framework (see later discussion of aerosol models, Sect.…”

Section: Definition Of Acidity In Terms Of the Phmentioning

confidence: 99%

“…Conversions among pH values calculated using different concentration scales is necessary to compare model predictions and to report acidity on a consistent basis. Generally, formulae for the conversion of pH are derived based upon the equivalence of the chemical potentials of solution entities irrespective of concentration scale (see, for example, Robinson and Stokes, 2002). The conversions to pH from the equivalent values on the mole fraction and molarity scales are given below, and the derivations are given in the Supplement (Sect.…”

Section: Symbol and Defining Expressionmentioning

confidence: 99%

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The acidity of atmospheric particles and clouds

et al. 2020

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Abstract. Acidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO3, NH3, HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale.

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Section: Definition Of Acidity In Terms Of the Phmentioning

confidence: 99%

Section: Symbol and Defining Expressionmentioning

confidence: 99%

The acidity of atmospheric particles and clouds

et al. 2020

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“…Semiquantification methods in some research showed that OSs accounted for 4–30% of organic matter (OM) (Hawkins et al, 2010; Surratt et al, 2008; Tolocka & Turpin, 2012) and 4–14% of total sulfate (Lukacs et al, 2009; Stone et al, 2012) in fine particles. Most previous work regarding OSs were examined in Europe (Frossard et al, 2011; Iinuma et al, 2007; Kristensen & Glasius, 2011; Lukacs et al, 2009; Nguyen et al, 2014) and the United States (Glasius, Bering, et al, 2018; Hettiyadura et al, 2019; Hughes & Stone, 2019; Olson et al, 2011; Riva et al, 2015; Riva et al, 2019; Tolocka & Turpin, 2012), but only a few studies were conducted in Asia (Huang, Cao, et al, 2018; Ma et al, 2014; Stone et al, 2012; Wang, Ma, et al, 2019), especially in China.…”

Section: Introductionmentioning

confidence: 99%

Molecular Characterization of Organosulfates in Highly Polluted Atmosphere Using Ultra‐High‐Resolution Mass Spectrometry

et al. 2020

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Organosulfates (OSs) have recently been observed to be a potentially important constituent of secondary organic aerosol (SOA); however, their molecular characterization in highly polluted atmospheres has not been probed in detail. This study thoroughly presents the characterization of OSs in polluted air and demonstrates their seasonal and diurnal variations, formation mechanisms, and contributions to organic aerosol. Atmospheric PM 2.5 samples were collected from an urban Shanghai site across the winter and summer of 2017. OSs were characterized by ultra-high-performance liquid chromatography (UHPLC) coupled with Orbitrap mass spectrometry (MS). Based on exact mass formulae in conjunction with previous chamber studies, hundreds of sulfur-containing compounds were tentatively identified as OSs. The number and abundance of OSs increased significantly during pollution episodes. The OSs in the clean aerosol samples were dominant in biogenic products, whereas the OSs in the polluted winter samples had distinctive anthropogenic characteristics. Aromatics and long-chain alkanes from anthropogenic emissions might be their precursors. By using synthesized standards, the total concentrations of 14 quantified OSs ranged 21.6-161 ng m −3 in summer and 5.85-84.3 ng m −3 in winter, respectively. Among these OSs, glycolic acid sulfate was the most abundant species (1.13-122 ng m −3 ). Further analysis of their seasonal and diurnal variations suggests possible contributions from multiple formation mechanisms, including acid-catalyzed and NO 3 -initiated oxidation reactions. Our results highlight that increased anthropogenic pollutant emissions (e.g., NO x and SO 2 ) can significantly enhance the SOA burden in biogenically influenced urban areas.

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“…Primary organic PM 2.5 is treated as inert in EASIUR, and secondary organic aerosol (SOA) is neglected because of the rapidly evolving understanding and representation of SOA formation in chemical transport models 20 . Anthropogenic emissions generally increase SOA through both volatile organic compounds (VOC) emissions and by enhancing the production of SOA from biogenic sources 48,49 . Therefore, the present analysis most likely underestimates the total mortality cost of PM 2.5 pollution, and omits the effects on SOA from other precursors such as NO x and effects of VOC emissions.…”

Section: Discussionmentioning

confidence: 99%

Air pollution control strategies directly limiting national health damages in the US

West

Smith

et al. 2020

Nat Commun

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Exposure to fine particulate matter (PM 2.5 ) from fuel combustion significantly contributes to global and US mortality. Traditional control strategies typically reduce emissions for specific air pollutants and sectors to maintain pollutant concentrations below standards. Here we directly set national PM 2.5 mortality cost reduction targets within a global human-earth system model with US state-level energy systems, in scenarios to 2050, to identify endogenously the control actions, sectors, and locations that most cost-effectively reduce PM 2.5 mortality. We show that substantial health benefits can be cost-effectively achieved by electrifying sources with high primary PM 2.5 emission intensities, including industrial coal, building biomass, and industrial liquids. More stringent PM 2.5 reduction targets expedite the phaseout of high emission intensity sources, leading to larger declines in major pollutant emissions, but very limited co-benefits in reducing CO 2 emissions. Control strategies limiting health damages achieve the greatest emission reductions in the East North Central and Middle Atlantic states.

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Increasing Isoprene Epoxydiol-to-Inorganic Sulfate Aerosol Ratio Results in Extensive Conversion of Inorganic Sulfate to Organosulfur Forms: Implications for Aerosol Physicochemical Properties

Cited by 137 publications

References 112 publications

The acidity of atmospheric particles and clouds

The acidity of atmospheric particles and clouds

Molecular Characterization of Organosulfates in Highly Polluted Atmosphere Using Ultra‐High‐Resolution Mass Spectrometry

Air pollution control strategies directly limiting national health damages in the US

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