The heterogeneous reactivity of gaseous nitric acid on authentic mineral dust samples, and on individual mineral and clay mineral components

Hänisch, F.; Crowley, John N.

doi:10.1039/b101700o

Cited by 89 publications

(115 citation statements)

References 17 publications

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“…Estimates for uptake on dry calcite range from 10 −4 to 0.1 for γ (HNO 3 ) (Goodman et al, 2000; Hanisch and Crowley, 2001), and 10 −4 to 4×10 −2 for γ (SO 2 ) (Usher et al, 2002;Ullerstam et al, 2003;Adams et al, 2005). Studies also show a marked increase in uptake rate with relative humidity for calcite, as uptake of water leads to enhanced ion mobility at the dust surface (Al-Hosney and Grassian, 2005;Vlasenko et al, 2006;Baltrusaitis et al, 2007a;Preszler-Prince et al, 2007;Liu et al, 2008).…”

Section: Acid Gas Uptake On Dustmentioning

confidence: 95%

“…We exclude direct uptake of ozone on dust, because the DC8 data show no significant negative correlation of ozone and dust (see discussion below). Laboratory studies indicate that uptake of ozone on dust is slow and subject to surface passivation (Hanisch and Crowley, 2003;Mogili et al, 2006). We also neglect particle coagulation since most studies of Asian outflow indicate that urban and dust aerosols are largely externally mixed (Mori et al, 2003;Maxwell-Meier et al, 2004;Tang et al, 2004;Song et al, 2005).…”

Section: Acid Gas Uptake On Dustmentioning

confidence: 99%

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Impact of mineral dust on nitrate, sulfate, and ozone in transpacific Asian pollution plumes

et al. 2010

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Abstract. We use a 3-D global chemical transport model (GEOS-Chem) to interpret aircraft observations of nitrate and sulfate partitioning in transpacific dust plumes during the INTEX-B campaign of April-May 2006. The model includes explicit transport of size-resolved mineral dust and its alkalinity, nitrate, and sulfate content. The observations show that particulate nitrate is primarily associated with dust, sulfate is primarily associated with ammonium, and Asian dust remains alkaline across the Pacific. This can be reproduced in the model by using a reactive uptake coefficient for HNO 3 on dust (γ (HNO 3 ) ∼10 −3 ) much lower than commonly assumed in models and possibly reflecting limitation of uptake by dust dissolution. The model overestimates gasphase HNO 3 by a factor of 2-3, typical of previous model studies; we show that this cannot be corrected by uptake on dust. We find that the fraction of aerosol nitrate on dust in the model increases from ∼30% in fresh Asian outflow to 80-90% over the Northeast Pacific, reflecting in part the volatilization of ammonium nitrate and the resulting transfer of nitrate to the dust. Consumption of dust alkalinity by uptake of acid gases in the model is slow relative to the lifetime of dust against deposition, so that dust does not acidify (at least not in the bulk). This limits the potential for dust iron released by acidification to become bio-available upon dust deposition. Observations in INTEX-B show no detectable Correspondence to: T. D. Fairlie (t.d.fairlie@nasa.gov) ozone depletion in Asian dust plumes, consistent with the model. Uptake of HNO 3 by dust, suppressing its recycling to NO x , reduces Asian pollution influence on US surface ozone in the model by 10-15% or up to 1 ppb.

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Section: Acid Gas Uptake On Dustmentioning

confidence: 95%

Section: Acid Gas Uptake On Dustmentioning

confidence: 99%

Impact of mineral dust on nitrate, sulfate, and ozone in transpacific Asian pollution plumes

et al. 2010

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“…The experimental set-up has been described in detail before (Hanisch and Crowley, 2001), and only salient features and modifications are reproduced here. The gas-mixing facility, Knudsen reactor and mass spectrometer are shown schematically in Fig.…”

Section: Methodsmentioning

confidence: 99%

“…tion (Hanisch and Crowley, 2001). They are listed in Table 1, together with other relevant Knudsen reactor parameters.…”

Section: Knudsen Reactor / Mass Spectrometermentioning

confidence: 99%

Ozone decomposition on Saharan dust: an experimental investigation

2003

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Abstract. The heterogeneous reaction between O 3 and authentic Saharan dust surfaces was investigated in a Knudsen reactor at ≈ 296 K. O 3 was destroyed on the dust surface and O 2 was formed with conversion efficiencies of 1.0 and 1.3 molecules O 2 per O 3 molecule destroyed for unheated and heated samples, respectively. No O 3 desorbed from exposed dust samples, showing that the uptake was irreversible. The uptake coefficients for the irreversible destruction of O 3 on (unheated) Saharan dust surfaces depended on the O 3 concentration and varied between 3.5 × 10 −4 and 5.5 × 10 −6 for the initial uptake coefficient (γ 0 ≈ 3 × 10 −5 at 30 ppbv O 3 STP) and between 4.8 × 10 −5 and 2.2 × 10 −6 for the steady-state uptake coefficient (γ ss ≈ 7 × 10 −6 at 30 ppbv O 3 STP). At very high O 3 concentrations the surface was deactivated, and O 3 uptake ceased after a certain exposure period. Sample re-activation (i.e. de-passivation) was found to occur over periods of hours, after exposure to O 3 had ceased, suggesting that re-activation processes play a role both in the laboratory and in the atmosphere.

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“…[30] We also considered in this work the irreversible uptake of HNO 3 on mineral dust with a g = 0.1 as in the works by Liao et al [2004], Liao and Seinfeld [2005], and Bauer et al [2004] following the recommendation of Hanisch and Crowley [2001]. NO 3 uptake on mineral dust has been also reported.…”

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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The heterogeneous reactivity of gaseous nitric acid on authentic mineral dust samples, and on individual mineral and clay mineral components

Cited by 89 publications

References 17 publications

Impact of mineral dust on nitrate, sulfate, and ozone in transpacific Asian pollution plumes

Impact of mineral dust on nitrate, sulfate, and ozone in transpacific Asian pollution plumes

Ozone decomposition on Saharan dust: an experimental investigation

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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