Heterogeneous reactions of soot aerosols with nitrogen dioxide and nitric acid: atmospheric chamber and Knudsen cell studies

Prince, A. Preszler; Wade, Jennifer L.; Grassian, Vicki H.; Kleiber, P. D.; Young, Mark A.

doi:10.1016/s1352-2310(02)00626-x

Cited by 62 publications

(62 citation statements)

References 19 publications

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“…The difference was explained by a surface reaction which takes place only at high HNO 3 concentrations for multilayer coverage of adsorbed HNO 3 (Choi and Leu, 1998). This is in accordance with other studies of Reaction (2) in which the formation of NO x was observed for very high HNO 3 concentrations (Disselkamp et al, 2000;Prince et al, 2002;Rogaski et al, 1997). However, in a very recent study of Salgado Muñoz and Rossi (2002) an irreversible reaction of HNO 3 with soot was observed also for low reactant concentrations.…”

Section: Introductionsupporting

confidence: 93%

“…formation of NO and NO 2 only for high HNO 3 concentrations, is in excellent agreement with nearly all studies of this reaction. In these studies no product formation was observed for low reactant concentrations (Aubin and Abbatt, 2003;Choi and Leu, 1998;Longfellow et al, 2000;Saathoff et al, 2001;Seisel et al, 2000), whereas the formation of NO x was observed for high reactant concentrations (Choi and Leu, 1998;Disselkamp et al, 2000;Prince et al, 2002;Rogaski et al, 1996). In addition, the absence of any HONO formation for Reaction (2) is in good agreement with the study of Aubin and Abbatt (2003), although the authors could not determine the upper limit of the product yield.…”

Section: Reaction Of Hno 3 With Soot Surfacesmentioning

confidence: 94%

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Heterogeneous conversion of NO2 and NO on HNO3 treated soot surfaces: atmospheric implications

Kleffmann

Wiesen

2005

Atmos. Chem. Phys.

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Abstract. In the present study, the heterogeneous conversion of nitrogen oxide (NO) and nitrogen dioxide (NO 2 ) was studied at atmospheric humidity levels on flame soot surfaces treated with gaseous nitric acid (HNO 3 ). In addition, the heterogeneous reaction of HNO 3 on soot was investigated at atmospheric humidity.For the treatment of soot by pure HNO 3 only reversible uptake with a surface coverage of ∼1-2×10 14 HNO 3 cm −2 was observed for HNO 3 mixing ratios in the range 250-800 ppbv. Only for higher HNO 3 mixing ratios of >800 ppbv the formation of NO and NO 2 was observed. The results were not affected by the addition of NO. In none of the experiments with HNO 3 the formation of nitrous acid (HONO) was observed. For HNO 3 mixing ratios <600 ppbv the upper limit yields for HONO, NO 2 and NO were found to be <0.2%, <0.5% and <1%, respectively. Compared to untreated soot, the product formation of the reaction of NO 2 with soot was not significantly affected when the soot surface was treated with gaseous HNO 3 prior to the experiment. Only for high surface coverage of HNO 3 the formation of HONO was suppressed in the initial phase of the reaction, probably caused by the blocking of active sites by adsorbed HNO 3 .Under the assumption that the experimental findings for the used model flame soot can be extrapolated to atmospheric soot particles, the results show that the reactions of HNO 3 and HNO 3 +NO on soot surfaces are unimportant for a "renoxification" of the atmosphere and do not represent an atmospheric HONO source. In addition, the integrated HONO yield of ca. 10 14 cm −2 in the reaction of NO 2 with soot is not significantly influenced by simulated atmospheric processing of the soot surface by HNO 3 , and is still too small to explain HONO formation in the atmosphere.

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Section: Introductionsupporting

confidence: 93%

Section: Reaction Of Hno 3 With Soot Surfacesmentioning

confidence: 94%

Heterogeneous conversion of NO2 and NO on HNO3 treated soot surfaces: atmospheric implications

Kleffmann

Wiesen

2005

Atmos. Chem. Phys.

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“…High sulfur and nitrogen concentrations on the surfaces of the accumulation-mode particles also suggest that the reactive uptake of NO x and SO 2 was quite feasible. Chemical reactions could further proceed among these adsorbed species (Prince et al 2002;Vander Wal et al 2011). …”

Section: Carbon Chemical Statesmentioning

confidence: 99%

Surface Chemical Composition of Size-Fractionated Urban Walkway Aerosols Determined by X-Ray Photoelectron Spectroscopy

Cheng

Weng

et al. 2013

Aerosol Science and Technology

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Most aerosol chemical characterization studies to date involve bulk particle analysis. The surface chemical and physical properties of aerosol particles have rarely been analyzed, despite the particles' potential health impacts and interactions with gas in the atmosphere. Aerosol particles ranging from 0.056 to 10 μm in size collected using a 10-stage impactor sampler from a busy walkway in a downtown area of Hong Kong were analyzed using X-ray photoelectron spectroscopy (XPS), a technique providing both elemental and chemical state information about the particle surfaces. Six key elements were detected: nitrogen (N), sulfur (S), calcium (Ca), silicon (Si), oxygen (O), and carbon (C). Carbon was the dominant species on the surfaces of all particles regardless of their sizes. A higher carbon concentration was found on the surfaces of the 0.056-0.32 μm particles. The N, Si, Ca, and O concentrations were higher on the surface of the 3.2-10 μm particles than in the smaller size fractions. Sulfur was mainly found on the surface of the 0.32-1.8 μm particles. High-resolution scans of C, N, and S were obtained to provide chemical state information about these elements. Aromatic C-H and aliphatic C-H were found to be the major carbon chemical states. Fullerenic carbon was detected on the surfaces of the finest (0.056-0.32 μm) particles. Oxygen-and nitrogen-containing organics were found on the surfaces of the 0.32-1.8 μm particles. Sulfur was present in the form of sulfates as expected. Ammonium salts, amide, and nitrate were found to form especially on the surfaces of aerosol particles in the nucleation, accumulation, and coarse modes, respectively. Silicates and carbonates were only discovered on the surfaces of coarse-mode particles (3.2-10 μm). The results suggest that both the chemical

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“…Although high emission ratios of HONO have been detected in laboratory fires Veres et al, 2010), the mixing ratio of HONO in aged BB plumes is expected to be relatively independent of its direct emissions due to the rapid dilution and photolysis for primary HONO during atmospheric transport. Soot particles, as one major component in BB plumes, have been demonstrated to be an effective media to convert NO 2 to HONO Aumont et al, 1999;Prince et al, 2002;Kleffmann and Wiesen, 2005;Aubin and Abbatt, 2007), especially in the case that aged soot particles can be re-activated in the present of light (Monge et al, 2010) and play a continuous role in the HONO chemistry. These processes may significantly influence the HONO chemistry during a BB period, but their exact roles are rarely demonstrated in the real atmosphere, especially when BB aerosols are mixed with anthropogenic pollutants.…”

Section: Introductionmentioning

confidence: 99%

Influence of biomass burning plumes on HONO chemistry in eastern China

et al. 2015

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Abstract. Nitrous acid (HONO) plays a key role in atmospheric chemistry by influencing the budget of hydroxyl radical (OH). In this study, a two-month measurement of HONO and related quantities were analyzed during a biomass burning season in 2012 at a suburban site in the western Yangtze River delta, eastern China. An overall high HONO concentration with the mean value of 0.76 ppbv (0.01 ppbv to 5.95 ppbv) was observed. During biomass burning (BB) periods, both HONO concentration and HONO/NO 2 ratio were enhanced significantly (more than a factor of 2, p<0.01) compared with non-biomass burning (non-BB) periods. A correlation analysis showed that the HONO in BB plumes was more correlated with nitrogen dioxide (NO 2 ) than that with potassium (a tracer of BB). Estimation by the method of potassium tracing suggests a maximum contribution of 17 ± 12 % from BB emission to the observed HONO concentrations, and the other over 80 % of the observed nighttime HONO concentrations during BB periods were secondarily produced by the heterogeneous conversion of NO 2 . The NO 2 -to-HONO conversion rate (C HONO ) in BB plumes was almost twice as that in non-BB plumes (0.0062 hr −1 vs. 0.0032 hr −1 ). Given that the residence time of the BB air masses was lower than that of non-BB air masses, these results suggest BB aerosols have higher NO 2 conversion potentials to form HONO than non-BB aerosols. A further analysis based on comparing the surface area at similar particle mass levels and HONO/NO 2 ratios at similar surface area levels suggested larger specific surface areas and higher NO 2 conversion efficiencies of BB aerosols. A mixed plume of BB and anthropogenic fossil fuel (FF) emissions was observed on 10 June with even higher HONO concentrations and HONO/NO 2 ratios. The strong HONO production potential (high HONO/NO 2 to PM 2.5 ratio) was accompanied with a high sulfate concentration in this plume, suggesting a promotion of mixed aerosols to the HONO formation. In summary, our study suggests an important role of BB in atmospheric chemistry by affecting the HONO budget. This can be especially important in eastern China, where agricultural burning plumes are inevitably mixed with urban and industrial pollution.

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Heterogeneous reactions of soot aerosols with nitrogen dioxide and nitric acid: atmospheric chamber and Knudsen cell studies

Cited by 62 publications

References 19 publications

Heterogeneous conversion of NO<sub>2</sub> and NO on HNO<sub>3</sub> treated soot surfaces: atmospheric implications

Heterogeneous conversion of NO<sub>2</sub> and NO on HNO<sub>3</sub> treated soot surfaces: atmospheric implications

Surface Chemical Composition of Size-Fractionated Urban Walkway Aerosols Determined by X-Ray Photoelectron Spectroscopy

Influence of biomass burning plumes on HONO chemistry in eastern China

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Heterogeneous reactions of soot aerosols with nitrogen dioxide and nitric acid: atmospheric chamber and Knudsen cell studies

Cited by 62 publications

References 19 publications

Heterogeneous conversion of NO&lt;sub&gt;2&lt;/sub&gt; and NO on HNO&lt;sub&gt;3&lt;/sub&gt; treated soot surfaces: atmospheric implications

Heterogeneous conversion of NO&lt;sub&gt;2&lt;/sub&gt; and NO on HNO&lt;sub&gt;3&lt;/sub&gt; treated soot surfaces: atmospheric implications

Surface Chemical Composition of Size-Fractionated Urban Walkway Aerosols Determined by X-Ray Photoelectron Spectroscopy

Influence of biomass burning plumes on HONO chemistry in eastern China

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Product

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Heterogeneous conversion of NO<sub>2</sub> and NO on HNO<sub>3</sub> treated soot surfaces: atmospheric implications

Heterogeneous conversion of NO<sub>2</sub> and NO on HNO<sub>3</sub> treated soot surfaces: atmospheric implications