Effects of aerosols on tropospheric oxidants : A global model study
Identifieur interne : 000219 ( PascalFrancis/Corpus ); précédent : 000218; suivant : 000220Effects of aerosols on tropospheric oxidants : A global model study
Auteurs : XUEXI TIE ; Guy Brasseur ; Louisa Emmons ; Larry Horowitz ; Douglas KinnisonSource :
- Journal of geophysical research [ 0148-0227 ] ; 2001.
Descripteurs français
- Pascal (Inist)
- Aérosol, Troposphère, Oxydant, Suie, Distribution planétaire, Azote pentaoxyde, Carbone particulaire, Réaction surface, Réaction hétérogène, Variation saisonnière, Répartition altitudinale, Soufre dioxyde, Sulfate, Nuage, Gouttelette, Captation, Etude sur modèle, Hydrogène peroxyde, Radical hydroxyle, Radical hydroperoxyle.
English descriptors
- KwdEn :
- Aerosols, Altitudinal distribution, Clouds, Droplet, Heterogeneous reaction, Hydrogen peroxide, Hydroperoxy radicals, Hydroxyl radicals, Model study, Nitrogen pentoxide, Oxidant, Particulate carbon, Planetary distribution, Seasonal variation, Soot, Sulfates, Sulfur dioxide, Surface reaction, Troposphere, Uptake.
Abstract
The global distributions of sulfate and soot particles in the atmosphere are calculated, and the effect of aerosol particles on tropospheric oxidants is studied using a global chemical/transport/ aerosol model. The model is developed in the framework of the National Center for Atmospheric Research (NCAR) global three-dimensional chemical/transport model (Model for Ozone and Related Chemical Tracers (MOZART)) In addition to the gas-phase photochemistry implemented in the MOZART model, the present study also accounts for the formation of sulfate and black carbon aerosols as well as for heterogeneous reactions on particles. The simulated global sulfate aerosol distributions and seasonal variation are compared with observations. The seasonal variation of sulfate aerosols is in agreement with measurements, except in the Arctic region. The calculated vertical profiles of sulfate aerosol agree well with the observations over North America. In the case of black carbon the calculated surface distribution is in fair agreement with observations. The effects of aerosol formation and heterogeneous reactions on the surface of sulfate aerosols are studied. The model calculations show the following: (1) The concentration of H2O2 is reduced when sulfate aerosols are formed due to the reaction of SO2 + H2O2 in cloud droplets. The gas-phase reaction SO2 + OH converts OH to HO2, but the reduction of OH and enhancement of HO2 are insignificant (< 3%). (2) The heterogeneous reaction of HO2 on the surface of sulfate aerosols produces up to 10% reduction of hydroperoxyl radical (HO2) with an uptake coefficient of 0.2. However, this uptake coefficient could be overestimated, and the results should be regard as an upper limit estimation. (3) The N2O5 reaction on the surface of sulfate aerosols leads to an 80% reduction of NOx at middle to high latitudes during winter. Because ozone production efficiency is low in winter, ozone decreases by only 10% as a result of this reaction. However, during summer the N2O5reaction reduces NOx by 15% and O3 by 8-10% at middle to high latitudes. (4) The heterogeneous reaction of CH2O on sulfate aerosols with an upper limit uptake coefficient (y = 0.01) leads to an 80 to 90% decrease in CH2O and 8 to 10% reduction of HO2 at middle to high latitudes during winter. Many uncertainties remain in our understanding of heterogeneous chemical processes and in the estimate of kinetic parameters. This model study should therefore be regarded as exploratory and subject to further improvements before final conclusions can be made.
Notice en format standard (ISO 2709)
Pour connaître la documentation sur le format Inist Standard.
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Format Inist (serveur)
NO : | PASCAL 02-0060291 INIST |
---|---|
ET : | Effects of aerosols on tropospheric oxidants : A global model study |
AU : | XUEXI TIE; BRASSEUR (Guy); EMMONS (Louisa); HOROWITZ (Larry); KINNISON (Douglas) |
AF : | National Center for Atmospheric Research/Boulder, Colorado/Etats-Unis (1 aut., 2 aut., 3 aut., 5 aut.); Geophysical Fluid Dynamics Laboratory, Princeton University./Princeton, New Jersey/Etats-Unis (4 aut.) |
DT : | Publication en série; Niveau analytique |
SO : | Journal of geophysical research; ISSN 0148-0227; Etats-Unis; Da. 2001; Vol. 106; No. D19; Pp. 22931-22964; Bibl. 1 p.3/4 |
LA : | Anglais |
EA : | The global distributions of sulfate and soot particles in the atmosphere are calculated, and the effect of aerosol particles on tropospheric oxidants is studied using a global chemical/transport/ aerosol model. The model is developed in the framework of the National Center for Atmospheric Research (NCAR) global three-dimensional chemical/transport model (Model for Ozone and Related Chemical Tracers (MOZART)) In addition to the gas-phase photochemistry implemented in the MOZART model, the present study also accounts for the formation of sulfate and black carbon aerosols as well as for heterogeneous reactions on particles. The simulated global sulfate aerosol distributions and seasonal variation are compared with observations. The seasonal variation of sulfate aerosols is in agreement with measurements, except in the Arctic region. The calculated vertical profiles of sulfate aerosol agree well with the observations over North America. In the case of black carbon the calculated surface distribution is in fair agreement with observations. The effects of aerosol formation and heterogeneous reactions on the surface of sulfate aerosols are studied. The model calculations show the following: (1) The concentration of H2O2 is reduced when sulfate aerosols are formed due to the reaction of SO2 + H2O2 in cloud droplets. The gas-phase reaction SO2 + OH converts OH to HO2, but the reduction of OH and enhancement of HO2 are insignificant (< 3%). (2) The heterogeneous reaction of HO2 on the surface of sulfate aerosols produces up to 10% reduction of hydroperoxyl radical (HO2) with an uptake coefficient of 0.2. However, this uptake coefficient could be overestimated, and the results should be regard as an upper limit estimation. (3) The N2O5 reaction on the surface of sulfate aerosols leads to an 80% reduction of NOx at middle to high latitudes during winter. Because ozone production efficiency is low in winter, ozone decreases by only 10% as a result of this reaction. However, during summer the N2O5reaction reduces NOx by 15% and O3 by 8-10% at middle to high latitudes. (4) The heterogeneous reaction of CH2O on sulfate aerosols with an upper limit uptake coefficient (y = 0.01) leads to an 80 to 90% decrease in CH2O and 8 to 10% reduction of HO2 at middle to high latitudes during winter. Many uncertainties remain in our understanding of heterogeneous chemical processes and in the estimate of kinetic parameters. This model study should therefore be regarded as exploratory and subject to further improvements before final conclusions can be made. |
CC : | 001E02D06 |
FD : | Aérosol; Troposphère; Oxydant; Suie; Distribution planétaire; Azote pentaoxyde; Carbone particulaire; Réaction surface; Réaction hétérogène; Variation saisonnière; Répartition altitudinale; Soufre dioxyde; Sulfate; Nuage; Gouttelette; Captation; Etude sur modèle; Hydrogène peroxyde; Radical hydroxyle; Radical hydroperoxyle |
ED : | Aerosols; Troposphere; Oxidant; Soot; Planetary distribution; Nitrogen pentoxide; Particulate carbon; Surface reaction; Heterogeneous reaction; Seasonal variation; Altitudinal distribution; Sulfur dioxide; Sulfates; Clouds; Droplet; Uptake; Model study; Hydrogen peroxide; Hydroxyl radicals; Hydroperoxy radicals |
SD : | Aerosol; Troposfera; Oxidante; Hollín; Distribución planetaria; Nitrógeno pentaóxido; Carbono particular; Reacción superficie; Reacción heterogénea; Variación estacional; Distribución de altitud; Dióxido sulfúrico; Sulfato; Nube; Gotita; Captación; Estudio sobre modelo |
LO : | INIST-3144.354000099817060260 |
ID : | 02-0060291 |
Links to Exploration step
Pascal:02-0060291Le document en format XML
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<term>Heterogeneous reaction</term>
<term>Hydrogen peroxide</term>
<term>Hydroperoxy radicals</term>
<term>Hydroxyl radicals</term>
<term>Model study</term>
<term>Nitrogen pentoxide</term>
<term>Oxidant</term>
<term>Particulate carbon</term>
<term>Planetary distribution</term>
<term>Seasonal variation</term>
<term>Soot</term>
<term>Sulfates</term>
<term>Sulfur dioxide</term>
<term>Surface reaction</term>
<term>Troposphere</term>
<term>Uptake</term>
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<term>Suie</term>
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<term>Azote pentaoxyde</term>
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<term>Variation saisonnière</term>
<term>Répartition altitudinale</term>
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<term>Sulfate</term>
<term>Nuage</term>
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<term>Captation</term>
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<front><div type="abstract" xml:lang="en">The global distributions of sulfate and soot particles in the atmosphere are calculated, and the effect of aerosol particles on tropospheric oxidants is studied using a global chemical/transport/ aerosol model. The model is developed in the framework of the National Center for Atmospheric Research (NCAR) global three-dimensional chemical/transport model (Model for Ozone and Related Chemical Tracers (MOZART)) In addition to the gas-phase photochemistry implemented in the MOZART model, the present study also accounts for the formation of sulfate and black carbon aerosols as well as for heterogeneous reactions on particles. The simulated global sulfate aerosol distributions and seasonal variation are compared with observations. The seasonal variation of sulfate aerosols is in agreement with measurements, except in the Arctic region. The calculated vertical profiles of sulfate aerosol agree well with the observations over North America. In the case of black carbon the calculated surface distribution is in fair agreement with observations. The effects of aerosol formation and heterogeneous reactions on the surface of sulfate aerosols are studied. The model calculations show the following: (1) The concentration of H<sub>2</sub>
O<sub>2</sub>
is reduced when sulfate aerosols are formed due to the reaction of SO<sub>2</sub>
+ H<sub>2</sub>
O<sub>2</sub>
in cloud droplets. The gas-phase reaction SO<sub>2</sub>
+ OH converts OH to HO<sub>2</sub>
, but the reduction of OH and enhancement of HO<sub>2</sub>
are insignificant (< 3%). (2) The heterogeneous reaction of HO<sub>2</sub>
on the surface of sulfate aerosols produces up to 10% reduction of hydroperoxyl radical (HO<sub>2</sub>
) with an uptake coefficient of 0.2. However, this uptake coefficient could be overestimated, and the results should be regard as an upper limit estimation. (3) The N<sub>2</sub>
O<sub>5</sub>
reaction on the surface of sulfate aerosols leads to an 80% reduction of NO<sub>x</sub>
at middle to high latitudes during winter. Because ozone production efficiency is low in winter, ozone decreases by only 10% as a result of this reaction. However, during summer the N<sub>2</sub>
O<sub>5</sub>
reaction reduces NO<sub>x</sub>
by 15% and O<sub>3</sub>
by 8-10% at middle to high latitudes. (4) The heterogeneous reaction of CH<sub>2</sub>
O on sulfate aerosols with an upper limit uptake coefficient (y = 0.01) leads to an 80 to 90% decrease in CH<sub>2</sub>
O and 8 to 10% reduction of HO<sub>2</sub>
at middle to high latitudes during winter. Many uncertainties remain in our understanding of heterogeneous chemical processes and in the estimate of kinetic parameters. This model study should therefore be regarded as exploratory and subject to further improvements before final conclusions can be made.</div>
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<fC01 i1="01" l="ENG"><s0>The global distributions of sulfate and soot particles in the atmosphere are calculated, and the effect of aerosol particles on tropospheric oxidants is studied using a global chemical/transport/ aerosol model. The model is developed in the framework of the National Center for Atmospheric Research (NCAR) global three-dimensional chemical/transport model (Model for Ozone and Related Chemical Tracers (MOZART)) In addition to the gas-phase photochemistry implemented in the MOZART model, the present study also accounts for the formation of sulfate and black carbon aerosols as well as for heterogeneous reactions on particles. The simulated global sulfate aerosol distributions and seasonal variation are compared with observations. The seasonal variation of sulfate aerosols is in agreement with measurements, except in the Arctic region. The calculated vertical profiles of sulfate aerosol agree well with the observations over North America. In the case of black carbon the calculated surface distribution is in fair agreement with observations. The effects of aerosol formation and heterogeneous reactions on the surface of sulfate aerosols are studied. The model calculations show the following: (1) The concentration of H<sub>2</sub>
O<sub>2</sub>
is reduced when sulfate aerosols are formed due to the reaction of SO<sub>2</sub>
+ H<sub>2</sub>
O<sub>2</sub>
in cloud droplets. The gas-phase reaction SO<sub>2</sub>
+ OH converts OH to HO<sub>2</sub>
, but the reduction of OH and enhancement of HO<sub>2</sub>
are insignificant (< 3%). (2) The heterogeneous reaction of HO<sub>2</sub>
on the surface of sulfate aerosols produces up to 10% reduction of hydroperoxyl radical (HO<sub>2</sub>
) with an uptake coefficient of 0.2. However, this uptake coefficient could be overestimated, and the results should be regard as an upper limit estimation. (3) The N<sub>2</sub>
O<sub>5</sub>
reaction on the surface of sulfate aerosols leads to an 80% reduction of NO<sub>x</sub>
at middle to high latitudes during winter. Because ozone production efficiency is low in winter, ozone decreases by only 10% as a result of this reaction. However, during summer the N<sub>2</sub>
O<sub>5</sub>
reaction reduces NO<sub>x</sub>
by 15% and O<sub>3</sub>
by 8-10% at middle to high latitudes. (4) The heterogeneous reaction of CH<sub>2</sub>
O on sulfate aerosols with an upper limit uptake coefficient (y = 0.01) leads to an 80 to 90% decrease in CH<sub>2</sub>
O and 8 to 10% reduction of HO<sub>2</sub>
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<s5>34</s5>
</fC03>
<fC03 i1="08" i2="X" l="SPA"><s0>Reacción superficie</s0>
<s5>34</s5>
</fC03>
<fC03 i1="09" i2="X" l="FRE"><s0>Réaction hétérogène</s0>
<s5>35</s5>
</fC03>
<fC03 i1="09" i2="X" l="ENG"><s0>Heterogeneous reaction</s0>
<s5>35</s5>
</fC03>
<fC03 i1="09" i2="X" l="SPA"><s0>Reacción heterogénea</s0>
<s5>35</s5>
</fC03>
<fC03 i1="10" i2="X" l="FRE"><s0>Variation saisonnière</s0>
<s5>36</s5>
</fC03>
<fC03 i1="10" i2="X" l="ENG"><s0>Seasonal variation</s0>
<s5>36</s5>
</fC03>
<fC03 i1="10" i2="X" l="SPA"><s0>Variación estacional</s0>
<s5>36</s5>
</fC03>
<fC03 i1="11" i2="X" l="FRE"><s0>Répartition altitudinale</s0>
<s5>37</s5>
</fC03>
<fC03 i1="11" i2="X" l="ENG"><s0>Altitudinal distribution</s0>
<s5>37</s5>
</fC03>
<fC03 i1="11" i2="X" l="SPA"><s0>Distribución de altitud</s0>
<s5>37</s5>
</fC03>
<fC03 i1="12" i2="X" l="FRE"><s0>Soufre dioxyde</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>38</s5>
</fC03>
<fC03 i1="12" i2="X" l="ENG"><s0>Sulfur dioxide</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>38</s5>
</fC03>
<fC03 i1="12" i2="X" l="SPA"><s0>Dióxido sulfúrico</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>38</s5>
</fC03>
<fC03 i1="13" i2="X" l="FRE"><s0>Sulfate</s0>
<s2>NA</s2>
<s5>39</s5>
</fC03>
<fC03 i1="13" i2="X" l="ENG"><s0>Sulfates</s0>
<s2>NA</s2>
<s5>39</s5>
</fC03>
<fC03 i1="13" i2="X" l="SPA"><s0>Sulfato</s0>
<s2>NA</s2>
<s5>39</s5>
</fC03>
<fC03 i1="14" i2="X" l="FRE"><s0>Nuage</s0>
<s5>40</s5>
</fC03>
<fC03 i1="14" i2="X" l="ENG"><s0>Clouds</s0>
<s5>40</s5>
</fC03>
<fC03 i1="14" i2="X" l="SPA"><s0>Nube</s0>
<s5>40</s5>
</fC03>
<fC03 i1="15" i2="X" l="FRE"><s0>Gouttelette</s0>
<s5>41</s5>
</fC03>
<fC03 i1="15" i2="X" l="ENG"><s0>Droplet</s0>
<s5>41</s5>
</fC03>
<fC03 i1="15" i2="X" l="SPA"><s0>Gotita</s0>
<s5>41</s5>
</fC03>
<fC03 i1="16" i2="X" l="FRE"><s0>Captation</s0>
<s5>42</s5>
</fC03>
<fC03 i1="16" i2="X" l="ENG"><s0>Uptake</s0>
<s5>42</s5>
</fC03>
<fC03 i1="16" i2="X" l="SPA"><s0>Captación</s0>
<s5>42</s5>
</fC03>
<fC03 i1="17" i2="X" l="FRE"><s0>Etude sur modèle</s0>
<s5>45</s5>
</fC03>
<fC03 i1="17" i2="X" l="ENG"><s0>Model study</s0>
<s5>45</s5>
</fC03>
<fC03 i1="17" i2="X" l="SPA"><s0>Estudio sobre modelo</s0>
<s5>45</s5>
</fC03>
<fC03 i1="18" i2="3" l="FRE"><s0>Hydrogène peroxyde</s0>
<s2>NK</s2>
<s5>83</s5>
</fC03>
<fC03 i1="18" i2="3" l="ENG"><s0>Hydrogen peroxide</s0>
<s2>NK</s2>
<s5>83</s5>
</fC03>
<fC03 i1="19" i2="3" l="FRE"><s0>Radical hydroxyle</s0>
<s2>NK</s2>
<s5>84</s5>
</fC03>
<fC03 i1="19" i2="3" l="ENG"><s0>Hydroxyl radicals</s0>
<s2>NK</s2>
<s5>84</s5>
</fC03>
<fC03 i1="20" i2="3" l="FRE"><s0>Radical hydroperoxyle</s0>
<s2>NK</s2>
<s5>85</s5>
</fC03>
<fC03 i1="20" i2="3" l="ENG"><s0>Hydroperoxy radicals</s0>
<s2>NK</s2>
<s5>85</s5>
</fC03>
<fN21><s1>028</s1>
</fN21>
</pA>
</standard>
<server><NO>PASCAL 02-0060291 INIST</NO>
<ET>Effects of aerosols on tropospheric oxidants : A global model study</ET>
<AU>XUEXI TIE; BRASSEUR (Guy); EMMONS (Louisa); HOROWITZ (Larry); KINNISON (Douglas)</AU>
<AF>National Center for Atmospheric Research/Boulder, Colorado/Etats-Unis (1 aut., 2 aut., 3 aut., 5 aut.); Geophysical Fluid Dynamics Laboratory, Princeton University./Princeton, New Jersey/Etats-Unis (4 aut.)</AF>
<DT>Publication en série; Niveau analytique</DT>
<SO>Journal of geophysical research; ISSN 0148-0227; Etats-Unis; Da. 2001; Vol. 106; No. D19; Pp. 22931-22964; Bibl. 1 p.3/4</SO>
<LA>Anglais</LA>
<EA>The global distributions of sulfate and soot particles in the atmosphere are calculated, and the effect of aerosol particles on tropospheric oxidants is studied using a global chemical/transport/ aerosol model. The model is developed in the framework of the National Center for Atmospheric Research (NCAR) global three-dimensional chemical/transport model (Model for Ozone and Related Chemical Tracers (MOZART)) In addition to the gas-phase photochemistry implemented in the MOZART model, the present study also accounts for the formation of sulfate and black carbon aerosols as well as for heterogeneous reactions on particles. The simulated global sulfate aerosol distributions and seasonal variation are compared with observations. The seasonal variation of sulfate aerosols is in agreement with measurements, except in the Arctic region. The calculated vertical profiles of sulfate aerosol agree well with the observations over North America. In the case of black carbon the calculated surface distribution is in fair agreement with observations. The effects of aerosol formation and heterogeneous reactions on the surface of sulfate aerosols are studied. The model calculations show the following: (1) The concentration of H<sub>2</sub>
O<sub>2</sub>
is reduced when sulfate aerosols are formed due to the reaction of SO<sub>2</sub>
+ H<sub>2</sub>
O<sub>2</sub>
in cloud droplets. The gas-phase reaction SO<sub>2</sub>
+ OH converts OH to HO<sub>2</sub>
, but the reduction of OH and enhancement of HO<sub>2</sub>
are insignificant (< 3%). (2) The heterogeneous reaction of HO<sub>2</sub>
on the surface of sulfate aerosols produces up to 10% reduction of hydroperoxyl radical (HO<sub>2</sub>
) with an uptake coefficient of 0.2. However, this uptake coefficient could be overestimated, and the results should be regard as an upper limit estimation. (3) The N<sub>2</sub>
O<sub>5</sub>
reaction on the surface of sulfate aerosols leads to an 80% reduction of NO<sub>x</sub>
at middle to high latitudes during winter. Because ozone production efficiency is low in winter, ozone decreases by only 10% as a result of this reaction. However, during summer the N<sub>2</sub>
O<sub>5</sub>
reaction reduces NO<sub>x</sub>
by 15% and O<sub>3</sub>
by 8-10% at middle to high latitudes. (4) The heterogeneous reaction of CH<sub>2</sub>
O on sulfate aerosols with an upper limit uptake coefficient (y = 0.01) leads to an 80 to 90% decrease in CH<sub>2</sub>
O and 8 to 10% reduction of HO<sub>2</sub>
at middle to high latitudes during winter. Many uncertainties remain in our understanding of heterogeneous chemical processes and in the estimate of kinetic parameters. This model study should therefore be regarded as exploratory and subject to further improvements before final conclusions can be made.</EA>
<CC>001E02D06</CC>
<FD>Aérosol; Troposphère; Oxydant; Suie; Distribution planétaire; Azote pentaoxyde; Carbone particulaire; Réaction surface; Réaction hétérogène; Variation saisonnière; Répartition altitudinale; Soufre dioxyde; Sulfate; Nuage; Gouttelette; Captation; Etude sur modèle; Hydrogène peroxyde; Radical hydroxyle; Radical hydroperoxyle</FD>
<ED>Aerosols; Troposphere; Oxidant; Soot; Planetary distribution; Nitrogen pentoxide; Particulate carbon; Surface reaction; Heterogeneous reaction; Seasonal variation; Altitudinal distribution; Sulfur dioxide; Sulfates; Clouds; Droplet; Uptake; Model study; Hydrogen peroxide; Hydroxyl radicals; Hydroperoxy radicals</ED>
<SD>Aerosol; Troposfera; Oxidante; Hollín; Distribución planetaria; Nitrógeno pentaóxido; Carbono particular; Reacción superficie; Reacción heterogénea; Variación estacional; Distribución de altitud; Dióxido sulfúrico; Sulfato; Nube; Gotita; Captación; Estudio sobre modelo</SD>
<LO>INIST-3144.354000099817060260</LO>
<ID>02-0060291</ID>
</server>
</inist>
</record>
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