scholarly journals Reactive Oxygen Species Formed by Secondary Organic Aerosols in Water and Surrogate Lung Fluid

Author(s):  
Haijie Tong ◽  
Pascale S. J. Lakey ◽  
Andrea M. Arangio ◽  
Joanna Socorro ◽  
Fangxia Shen ◽  
...  
2017 ◽  
Vol 200 ◽  
pp. 251-270 ◽  
Author(s):  
Haijie Tong ◽  
Pascale S. J. Lakey ◽  
Andrea M. Arangio ◽  
Joanna Socorro ◽  
Christopher J. Kampf ◽  
...  

Mineral dust and secondary organic aerosols (SOA) account for a major fraction of atmospheric particulate matter, affecting climate, air quality and public health. How mineral dust interacts with SOA to influence cloud chemistry and public health, however, is not well understood. Here, we investigated the formation of reactive oxygen species (ROS), which are key species of atmospheric and physiological chemistry, in aqueous mixtures of SOA and mineral dust by applying electron paramagnetic resonance (EPR) spectrometry in combination with a spin-trapping technique, liquid chromatography-tandem mass spectrometry (LC-MS/MS), and a kinetic model. We found that substantial amounts of ROS including OH, superoxide as well as carbon- and oxygen-centred organic radicals can be formed in aqueous mixtures of isoprene, α-pinene, naphthalene SOA and various kinds of mineral dust (ripidolite, montmorillonite, kaolinite, palygorskite, and Saharan dust). The molar yields of total radicals were ∼0.02–0.5% at 295 K, which showed higher values at 310 K, upon 254 nm UV exposure, and under low pH (<3) conditions. ROS formation can be explained by the decomposition of organic hydroperoxides, which are a prominent fraction of SOA, through interactions with water and Fenton-like reactions with dissolved transition metal ions. Our findings imply that the chemical reactivity and aging of SOA particles can be enhanced upon interaction with mineral dust in deliquesced particles or cloud/fog droplets. SOA decomposition could be comparably important to the classical Fenton reaction of H2O2 with Fe2+ and that SOA can be the main source of OH radicals in aqueous droplets at low concentrations of H2O2 and Fe2+. In the human respiratory tract, the inhalation and deposition of SOA and mineral dust can also lead to the release of ROS, which may contribute to oxidative stress and play an important role in the adverse health effects of atmospheric aerosols in the Anthropocene.


2019 ◽  
Vol 53 (15) ◽  
pp. 8553-8562 ◽  
Author(s):  
Alessandro Manfrin ◽  
Sergey A. Nizkorodov ◽  
Kurtis T. Malecha ◽  
Gordon J. Getzinger ◽  
Kristopher McNeill ◽  
...  

2019 ◽  
Vol 53 (23) ◽  
pp. 13949-13958 ◽  
Author(s):  
Pratiti Home Chowdhury ◽  
Quanfu He ◽  
Raanan Carmieli ◽  
Chunlin Li ◽  
Yinon Rudich ◽  
...  

2021 ◽  
Author(s):  
Sophie Bogler ◽  
Nadine Borduas-Dedekind ◽  
Imad el Haddad ◽  
David Bell ◽  
Kaspar Dällenbach

&lt;p&gt;Singlet oxygen (&lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt;) is a reactive oxygen species that has recently gained attention as a competitive oxidant in the atmosphere. This excited state of molecular oxygen is formed by indirect photochemistry in the presence of chromophoric dissolved organic matter (DOM) as sensitizers, molecular oxygen and sunlight. The produced highly reactive intermediate &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;is then capable of oxidizing and degrading many organic atmospheric components, thereby affecting their lifetime in the atmosphere. Despite this influence on atmospheric fate, the spatiotemporal distribution of &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; in particular matter (PM) is currently unknown. We hypothesized that brown carbon in biomass burning organic aerosols emitted during winter in Switzerland would lead to higher &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; steady-state concentrations in PM compared to summer. Therefore, to advance atmospheric &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;research, we investigated the &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; sensitizing ability of organic aerosols sampled on 24-hour PM10 filters. Specifically, these filters were collected throughout 2013 in Frauenfeld and San Vittore in Switzerland, characterized as urban background and rural traffic measurement stations, respectively. We extracted the water-soluble organic components and quantified &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;steady state concentrations as well as &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; quantum yield. The quantum yield enhances the data intercomparison as this value shows the normalization of &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;production as a function of the rate of absorbance of the organic aerosols. In our ongoing efforts of expanding the spatiotemporal scale of our measurements, our results from Frauenfeld so far show a range between 0.38 &amp;#8211; 6.05 &amp;#183; 10&lt;sup&gt;-13 &lt;/sup&gt;M for &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;steady state concentrations and quantum yields up to 2.1&amp;#177; 0.5&lt;sup&gt;&lt;/sup&gt;%. In preliminary experiments, samples from the rural site San Vittore show similar values, with potentially higher values during periods of significant biomass burning contributions. The values underline &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt;&amp;#8217;s&lt;sub&gt;&lt;/sub&gt;potential importance for atmospheric processing, e.g. comparing to Manfrin et al. (ES&amp;T, 2019)&lt;sup&gt;1&lt;/sup&gt; who reported &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;steady state concentrations of 3 &amp;#177; 1 &amp;#183; 10&lt;sup&gt;-14 &lt;/sup&gt;M from secondary organic aerosols extracts. More importantly, the filter extracts analyzed thus far show a strong seasonal trend, with increased &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;values and higher variability in winter as compared to summer. This result corroborates the hypothesis that there is more chromophoric DOM present in winter, due to a higher fraction of brown carbon emitted e.g. in biomass burning for residential heating. To extend this analysis, we are currently correlating the results for &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;with molecular markers based on mass spectrometry data available from previous filter analysis provided by Daellenbach et al., (ACP, 2017)&lt;sup&gt;2&lt;/sup&gt;. Finding these correlations will enable the prediction of &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;sensitizing abilities of organic material present in the aerosols both qualitatively and quantitatively. In all, our work will help constrain the seasonal relevance of &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;photochemistry in the atmosphere.&lt;/p&gt;&lt;p&gt;&lt;strong&gt;References&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;1. Manfrin, A. et al. Reactive Oxygen Species Production from Secondary Organic Aerosols: The Importance of Singlet Oxygen. Environmental Science &amp; Technology 53, 8553&amp;#8211;8562 (2019).&lt;br&gt;2. Daellenbach, K. R. et al. Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment. Atmospheric Chemistry and Physics 17, 13265&amp;#8211;13282 (2017).&lt;/p&gt;


2015 ◽  
Vol 49 (7) ◽  
pp. 4646-4656 ◽  
Author(s):  
Vishal Verma ◽  
Ting Fang ◽  
Lu Xu ◽  
Richard E. Peltier ◽  
Armistead G. Russell ◽  
...  

2017 ◽  
Vol 17 (16) ◽  
pp. 9853-9868 ◽  
Author(s):  
Peter J. Gallimore ◽  
Brendan M. Mahon ◽  
Francis P. H. Wragg ◽  
Stephen J. Fuller ◽  
Chiara Giorio ◽  
...  

Abstract. The chemical composition of organic aerosols influences their impacts on human health and the climate system. Aerosol formation from gas-to-particle conversion and in-particle reaction was studied for the oxidation of limonene in a new facility, the Cambridge Atmospheric Simulation Chamber (CASC). Health-relevant oxidising organic species produced during secondary organic aerosol (SOA) formation were quantified in real time using an Online Particle-bound Reactive Oxygen Species Instrument (OPROSI). Two categories of reactive oxygen species (ROS) were identified based on time series analysis: a short-lived component produced during precursor ozonolysis with a lifetime of the order of minutes, and a stable component that was long-lived on the experiment timescale (∼ 4 h). Individual organic species were monitored continuously over this time using Extractive Electrospray Ionisation (EESI) Mass Spectrometry (MS) for the particle phase and Proton Transfer Reaction (PTR) MS for the gas phase. Many first-generation oxidation products are unsaturated, and we observed multiphase aging via further ozonolysis reactions. Volatile products such as C9H14O (limonaketone) and C10H16O2 (limonaldehyde) were observed in the gas phase early in the experiment, before reacting again with ozone. Loss of C10H16O4 (7-hydroxy limononic acid) from the particle phase was surprisingly slow. A combination of reduced C = C reactivity and viscous particle formation (relative to other SOA systems) may explain this, and both scenarios were tested in the Pretty Good Aerosol Model (PG-AM). A range of characterisation measurements were also carried out to benchmark the chamber against existing facilities. This work demonstrates the utility of CASC, particularly for understanding the reactivity and health-relevant properties of organic aerosols using novel, highly time-resolved techniques.


2017 ◽  
Author(s):  
Peter J. Gallimore ◽  
Brendan M. Mahon ◽  
Francis P. H. Wragg ◽  
Stephen J. Fuller ◽  
Chiara Giorio ◽  
...  

Abstract. The chemical composition of organic aerosols influences their impacts on human health and the climate system. Aerosol formation from gas-to-particle conversion and in-particle reaction was studied for the oxidation of limonene in a new facility, the Cambridge Atmospheric Simulation Chamber (CASC). Health-relevant oxidising organic species produced during SOA formation were quantified in real-time using an Online Particle-bound Reactive Oxygen Species Instrument (OPROSI). Two categories of reactive oxygen species (ROS) were identified based on time series analysis: a short-lived component produced during precursor ozonolysis with a lifetime on the order of minutes, and a stable component which was long-lived on the experiment timescale (~ 4 hours). Individual organic species were monitored continuously over this time using Extractive Electrospray Ionisation (EESI) Mass Spectrometry (MS) for the particle phase and Proton Transfer Reaction (PTR) MS for the gas phase. Many first generation oxidation products are unsaturated, and we observed multiphase aging via further ozonolysis reactions. Volatile products such as C9H14O (limonaketone) and C10H16O2 (limonaldehyde) were observed in the gas phase early in the experiment, before reacting again with ozone. Loss of C10H16O2 (7-hydroxy limononic acid) from the particle phase was surprisingly slow. A combination of reduced C=C reactivity and viscous particle formation (relative to other SOA systems) may explain this, and both scenarios were tested in the Pretty Good Aerosol Model (PG-AM). A range of characterisation measurements were also carried out to benchmark the chamber against existing facilities. This work demonstrates the utility of the CASC chamber, particularly for understanding the reactivity and health-relevant properties of organic aerosols using novel, highly time-resolved techniques.


2009 ◽  
pp. c3 ◽  
Author(s):  
Helena M. Cochemé ◽  
Michael P. Murphy

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