N2O5 hydrolysis on sub-micron organic aerosols: the effect of relative humidity, particle phase, and particle size

Thornton, Joel A.; Braban, Christine F.; Abbatt, Jonathan P. D.

doi:10.1039/b307498f

Cited by 222 publications

(403 citation statements)

References 38 publications

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“…The observed particle-phase ON group hydrolysis rate (Figure 5b) is consistent with the phase transition of SOA from solid to semisolid/liquid particles: The hydrolysis rate was ∼0 and 4 day −1 (corresponding to a lifetime of 6 h) for RH < 20% and > 40% experiments, respectively. The pronounced increase of hydrolysis rate at 40% RH also agrees with the hydrolysis loss rate of N 2 O 5 on organic particles, which is dependent on water concentration when RH < 50% and appears to be independent of water when RH is greater than 50% (Thornton et al 2003).…”

Section: Fig 3 Time-dependence Of (A) Rh (B) Temperature (C) Tmbsupporting

confidence: 69%

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Liu

Shilling

Song

et al. 2012

Aerosol Science and Technology

183

204

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Organonitrate (ON) groups are thought to be important substituents in secondary organic aerosols (SOAs). Model simulations and laboratory studies indicate a large fraction of ON groups in aerosol particles, but much lower quantities are observed in the atmosphere. Hydrolysis of ON groups in aerosol particles has been proposed recently to account for this discrepancy. To test this hypothesis, we simulated formation of ON molecules in a reaction chamber under a wide range of relative humidity (RH) (0 to 90%). The mass fraction of ON groups (5 to 20% for high-NO x experiments) consistently decreased with increasing RH, which was best explained by hydrolysis of ON groups at a rate of 4 day −1 (lifetime of 6 h) for reactions under RH greater than 20%. In addition, we found that secondary nitrogen-containing molecules absorb light, with greater absorption under dry and high-NO x conditions. This work provides the first evidence for particle-phase hydrolysis of ON groups, a process that could substantially reduce ON group concentration in atmospheric SOAs.

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Section: Fig 3 Time-dependence Of (A) Rh (B) Temperature (C) Tmbsupporting

confidence: 69%

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Liu

Shilling

Song

et al. 2012

Aerosol Science and Technology

183

204

View full text Add to dashboard Cite

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“…Note that γ N 2 O 5 values appeared to increase with rising relative humidity, which was also observed at other sites (X. Thornton et al, 2003). For example, γ N 2 O 5 values increased from 0.019 to 0.090 when RH increased from 21.1 % to 63.6 %.…”

Section: N 2 O 5 Uptake Coefficient and Clno 2 Production Yieldsupporting

confidence: 49%

“…However, the γ N 2 O 5 determined in our campaign was 1-2 or- ders of magnitude higher than obtained in the laboratory (Thornton et al, 2003) and also much higher than those in Hong Kong and Germany (Brown et al, 2016b;Phillips et al, 2016). We also found that the parameterized γ N 2 O 5 values (0.0014-0.012) determined from Eq.…”

Section: N 2 O 5 Uptake Coefficient and Clno 2 Production Yieldsupporting

confidence: 48%

“…N 2 O 5 exists in a rapid temperaturedependent thermal equilibrium with the nitrate radical (NO 3 ) -one of the most important oxidants at nighttime (Wayne et al, 1991). Although NO 3 and N 2 O 5 levels can be suppressed by the rapid titration of NO 3 against NO and volatile organic compounds (VOCs) in urban areas (Brown et al, 2003b), heterogeneous uptake by aerosol particles, fog, and cloud droplets is often found to be the major pathway for direct N 2 O 5 removal (Bertram and Thornton, 2009;Wagner et al, 2013;Brown et al, 2006;Chang et al, 2011;Thornton et al, 2003). N 2 O 5 can produce nitryl chloride (ClNO 2 ) on chloride-containing aerosols, which serves as an important reservoir of NO x (Finlayson-Pitts et al, 1989;Thornton et al, 2010;Phillips et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

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Production of N2O5 and ClNO2 in summer in urban Beijing, China

et al. 2018

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Abstract. The heterogeneous hydrolysis of dinitrogen pentoxide (N 2 O 5 ) has a significant impact on both nocturnal particulate nitrate formation and photochemistry on the following day through the photolysis of nitryl chloride (ClNO 2 ), yet these processes in highly polluted urban areas remain poorly understood. Here we present measurements of gas-phase Further analysis indicates that the fast N 2 O 5 loss in the nocturnal boundary layer in urban Beijing is mainly attributed to its indirect loss via NO 3 , for example through the reactions with volatile organic compounds and NO, while the contribution of the heterogeneous uptake of N 2 O 5 is comparably small (7-33 %). High ClNO 2 yields ranging from 0.10 to 0.35 were also observed, which might have important implications for air quality by affecting nitrate and ozone formation.

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“…For instance, the total gas-to-particle transfer rate of N 2 O 5 K N 2 O 5 is calculated as the sum of the specific K N 2 O 5 ,i x as follows: [29] We implemented the reactions of HO 2 , NO 2 , NO 3 on wet aerosol particles (e.g., all the soluble modes (NS, KS, AS, and CS) in the model, independently of their composition) with the uptake coefficients of 0.2, 10 À4 and 10 À3 , respectively, following Jacob [2000]. The uptake of N 2 O 5 on aerosol particles follows Evans and Jacob [2005] and Liao and Seinfeld [2005], i.e., different coefficients are used for sulfate [Kane et al, 2001;Hallquist et al, 2003], organic carbon [Thornton et al, 2003], black carbon [Sander et al, 2003], sea salt [Atkinson et al, 2004], and mineral dust [Bauer et al, 2004]. The O 3 uptake coefficient on mineral dust is set to 10 À5 following Bauer et al [2004].…”

Section: Heterogeneous Chemistrymentioning

confidence: 99%

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

et al. 2008

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[1] In this paper, we introduce the ECHAM5-HAMMOZ aerosol-chemistry-climate model that includes fully interactive simulations of Ox-NOx-hydrocarbons chemistry and of aerosol microphysics (including prognostic size distribution and mixing state of aerosols) implemented in the General Circulation Model ECHAM5. The photolysis rates used in the gas chemistry account for aerosol and cloud distributions and a comprehensive set of heterogeneous reactions is implemented. The model is evaluated with trace gas and aerosol observations provided by the TRACE-P aircraft experiment. Sulfate concentrations are well captured but black carbon concentrations are underestimated. The number concentrations, surface areas, and optical properties are reproduced fairly well near the surface but underestimated in the upper troposphere. CO concentrations are well reproduced in general while O 3 concentrations are overestimated by 10-20 ppbv. We find that heterogeneous chemistry significantly influences the regional and global distributions of a number of key trace gases. Heterogeneous reactions reduce the ozone surface concentrations by 18-23% over the TRACE-P region and the global annual mean O 3 burden by 7%. The annual global mean OH concentration decreases by 10% inducing a 7% increase in the global CO burden. Annual global mean HNO 3 surface concentration decreases by 15% because of heterogenous reaction on mineral dust. A comparison of our results to those from previous studies suggests that the choice of uptake coefficients for a given species is the critical parameter that determines the global impact of heterogeneous chemistry on a trace gas (rather than the description of aerosol properties and distributions). A prognostic description of the size distribution and mixing state of the aerosols is important, however, to account for the effect of heterogeneous chemistry on aerosols as further discussed in the second part of this two-part series.Citation: Pozzoli, L., I. Bey, S. Rast, M. G. Schultz, P. Stier, and J. Feichter (2008), Trace gas and aerosol interactions in the fully coupled model of aerosol-chemistry-climate ECHAM5-HAMMOZ: 1. Model description and insights from the spring 2001 TRACE-P experiment,

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N2O5 hydrolysis on sub-micron organic aerosols: the effect of relative humidity, particle phase, and particle size

Cited by 222 publications

References 38 publications

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Production of N<sub>2</sub>O<sub>5</sub> and ClNO<sub>2</sub> in summer in urban Beijing, China

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

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N2O5 hydrolysis on sub-micron organic aerosols: the effect of relative humidity, particle phase, and particle size

Cited by 222 publications

References 38 publications

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Production of N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt; and ClNO&lt;sub&gt;2&lt;/sub&gt; in summer in urban Beijing, China

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

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Production of N<sub>2</sub>O<sub>5</sub> and ClNO<sub>2</sub> in summer in urban Beijing, China