HONO Emissions from Soil Bacteria as a Major Source of Atmospheric Reactive Nitrogen

Oswald, R.; Behrendt, Thomas; Ermel, Michael; Wu, Dianming; Su, Hang; Cheng, Yafang; Breuninger, C.; Moravek, Alexander; Mougin, E.; Delon, Claire; Loubet, Benjamin; Pommerening‐Röser, Andreas; Sörgel, Matthias; Pöschl, Ulrich; Hoffmann, Thorsten; Andreae, Meinrat O.; Meixner, Franz X.; Trebs, Ivonne

doi:10.1126/science.1242266

Cited by 298 publications

(478 citation statements)

References 43 publications

(38 reference statements)

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“…Zhou et al (2011) claimed that significant HONO could be generated from nitrate photolysis processes on forest canopy surface by presenting observational data from a hardwood forest in Pellston, MI. Finally, HONO emission from soil bacteria is also proposed (Oswald et al, 2013). Oswald et al (2013) found differences as much as 2 orders of magnitude in HONO emissions from soil samples from different environments (e.g., pH and nutrient contents).…”

Section: Observational Resultsmentioning

confidence: 99%

“…Finally, HONO emission from soil bacteria is also proposed (Oswald et al, 2013). Oswald et al (2013) found differences as much as 2 orders of magnitude in HONO emissions from soil samples from different environments (e.g., pH and nutrient contents). In addition, as most of observations in the East Asia regions were conducted with ionchromatography-based methods, more direct HONO quantification techniques such as a chemical ionization mass spectrometry technique (Roberts et al, 2010) need to be used to characterize any potential interferences such a high NO x environment (e.g., N 2 O 5 ).…”

Section: Observational Resultsmentioning

confidence: 99%

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Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Kim

Lee³

et al. 2015

Atmos. Chem. Phys.

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Abstract. Rapid urbanization and economic development in East Asia in past decades has led to photochemical air pollution problems such as excess photochemical ozone and aerosol formation. Asian megacities such as Seoul, Tokyo, Shanghai, Guangzhou, and Beijing are surrounded by densely forested areas, and recent research has consistently demonstrated the importance of biogenic volatile organic compounds (VOCs) from vegetation in determining oxidation capacity in the suburban Asian megacity regions. Uncertainties in constraining tropospheric oxidation capacity, dominated by hydroxyl radical, undermine our ability to assess regional photochemical air pollution problems. We present an observational data set of CO, NO x , SO 2 , ozone, HONO, and VOCs (anthropogenic and biogenic) from Taehwa research forest (TRF) near the Seoul metropolitan area in early June 2012. The data show that TRF is influenced both by aged pollution and fresh biogenic volatile organic compound emissions. With the data set, we diagnose HO x (OH, HO 2 , and RO 2 ) distributions calculated using the University of Washington chemical box model (UWCM v2.1) with nearexplicit VOC oxidation mechanisms from MCM v3.2 (Master Chemical Mechanism). Uncertainty from unconstrained HONO sources and radical recycling processes highlighted in recent studies is examined using multiple model simulations with different model constraints. The results suggest that (1) different model simulation scenarios cause systematic differences in HO x distributions, especially OH levels (up to 2.5 times), and (2) radical destruction (HO 2 + HO 2 or HO 2 + RO 2 ) could be more efficient than radical recycling (RO 2 + NO), especially in the afternoon. Implications of the uncertainties in radical chemistry are discussed with respect to ozone-VOC-NO x sensitivity and VOC oxidation product formation rates. Overall, the NO x limited regime is assessed except for the morning hours (8 a.m. to 12 p.m. local standard time), but the degree of sensitivity can significantly vary depending on the model scenarios. The model results also suggest that RO 2 levels are positively correlated with oxygenated VOCs (OVOCs) production that is not routinely constrained by observations. These unconstrained OVOCs can cause higher-than-expected OH loss rates (missing OH reactivity) and secondary organic aerosol formation. The series of modeling experiments constrained by observations strongly urge observational constraint of the radical pool to enable precise understanding of regional photochemical pollution problems in the East Asian megacity region.

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Section: Observational Resultsmentioning

confidence: 99%

Section: Observational Resultsmentioning

confidence: 99%

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Kim

Lee³

et al. 2015

Atmos. Chem. Phys.

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“…Other aspects of chemistry that are often omitted include the full range of peroxy radical cross reactions (incomplete in even the MCM; Saunders et al, 2003); peroxy radical recycling from isoprene oxidation (e.g., Crounse et al, 2011;Peters et al, 2014), which some studies indicate can affect OH levels and VOC lifetimes over low-NO x forested areas (Archibald et al, 2010b(Archibald et al, , 2011Taraborrelli et al, 2012); nitryl chloride (ClNO 2 ), which has been found to be important in oxidative chemistry, particularly in coastal regions (e.g., Osthoff et al, 2008); and nitrous acid (HONO) formation other than from NO + OH (+M), including from other gas phase sources (Bejan et al, 2007: Li et al, 2008Li et al, 2014), bacteria (Oswald et al, 2013), aerosol reactions (Ammann et al, 1998Stemmler et al, 2007) and heterogeneous processes (Zhou et al, 2001;Stemmler et al, 2006;Su et al, 2011;Mao et al, 2013). In general, heterogeneous processes (Ravishankara, 1997;Jacob, 2000) are simulated in most models, although typically only for a few species (e.g., heterogeneous formation of N 2 O 5 and loss of HO 2 ) and with substantial variation in uptake coefficients, which can have notable effects on modeled abundances and chemical budgets (e.g., Evans and Jacob, 2005;Macintyre and Evans, 2010).…”

Section: Chemistrymentioning

confidence: 99%

Tropospheric Ozone Assessment Report: Assessment of global-scale model performance for global and regional ozone distributions, variability, and trends

Young

Naik

Fiore

et al. 2018

Elementa: Science of the Anthropocene

241

271

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The goal of the Tropospheric Ozone Assessment Report (TOAR) is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for the problem being addressed, whether biases can be tolerated or corrected, whether the model is appropriately constituted, and whether there is a way to satisfactorily quantify the uncertainty.

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“…Stemmler et al (2006Stemmler et al ( , 2007 found HONO formation on light-activated humic acid, and field studies showed that HONO formation correlates with aerosol surface area, NO 2 and solar radiation (Su et al, 2008;Reisinger, 2000;Costabile et al, 2010;Wong et al, 2012;Sörgel et al, 2015) and is increased during foggy periods (Notholt et al, 1992). Another proposed source of HONO is the soil, where it has been found to be co-emitted with NO by soil biological activities (Oswald et al, 2013;Su et al, 2011;Weber et al, 2015). In view of light-induced nitration of proteins and HONO formation by photolysis of nitrophenols, light-enhanced production of HONO on protein surfaces can be anticipated, which, to the best of our knowledge, has not been studied before.…”

Section: Introductionmentioning

confidence: 99%

Light-induced protein nitration and degradation with HONO emission

et al. 2017

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Abstract. Proteins can be nitrated by air pollutants (NO 2 ), enhancing their allergenic potential. This work provides insight into protein nitration and subsequent decomposition in the presence of solar radiation. We also investigated lightinduced formation of nitrous acid (HONO) from protein surfaces that were nitrated either online with instantaneous gas-phase exposure to NO 2 or offline by an efficient nitration agent (tetranitromethane, TNM). Bovine serum albumin (BSA) and ovalbumin (OVA) were used as model substances for proteins. Nitration degrees of about 1 % were derived applying NO 2 concentrations of 100 ppb under VIS/UV illuminated conditions, while simultaneous decomposition of (nitrated) proteins was also found during long-term (20 h) irradiation exposure. Measurements of gas exchange on TNMnitrated proteins revealed that HONO can be formed and released even without contribution of instantaneous heterogeneous NO 2 conversion. NO 2 exposure was found to increase HONO emissions substantially. In particular, a strong dependence of HONO emissions on light intensity, relative humidity, NO 2 concentrations and the applied coating thickness was found. The 20 h long-term studies revealed sustained HONO formation, even when concentrations of the intact (nitrated) proteins were too low to be detected after the gas exchange measurements. A reaction mechanism for the NO 2 conversion based on the Langmuir-Hinshelwood kinetics is proposed.

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HONO Emissions from Soil Bacteria as a Major Source of Atmospheric Reactive Nitrogen

Cited by 298 publications

References 43 publications

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Tropospheric Ozone Assessment Report: Assessment of global-scale model performance for global and regional ozone distributions, variability, and trends

Light-induced protein nitration and degradation with HONO emission

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