[化学]全球化模型研究气溶胶与对流层氧化剂.pdf

JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 106, NO. D19, PAGES 22,931-22,964,OCTOBER 16, 2001 Effects of aerosolson tropospheric oxidants A global model study Xuexi Tie, Guy Brasseur,•andLouisa Emmons NationalCenterfor AtmosphericResearch,Boulder,Colorado,USA Larry Horowitz GeophysicalFluid DynamicsLaboratory,PrincetonUniversity,Princeton,New Jersey,USA DouglasKinnison NationalCenterfor AtmosphericResearch,Boulder,Colorado,USA Abstract. The globaldistributionsof sulfateand sootparticlesin the atmosphereare calculated, andtheeffect of aerosolparticleson troposphericoxidantsis studiedusinga global chemical/transport/aerosolmodel.The model is developedin the frameworkof the National Centerfor AtmosphericResearch(NCAR) globalthree-dimensionalchemical/transportmodel (Model for OzoneandRelatedChemicalTracers(MOZART)). In additionto the gas-phase photochemistryimplementedin the MOZART model,the presentstudyalsoaccountsfor the formationof sulfateandblackcarbonaerosolsaswell asfor heterogeneousreactionson particles. The simulatedglobalsulfateaerosoldistributionsandseasonalvariationare comparedwith observations.The seasonalvariationof sulfateaerosolsis in agreementwith measurements,except in the Arctic region.The calculatedvertical profilesof sulfateaerosolagreewell with the observations over North America. In the case of black carbon the calculated surface distribution is in fair agreementwith observations.The effectsof aerosolformationand heterogeneousreactions on the surfaceof sulfateaerosolsare studied.The modelcalculationsshowthe following (1) The concentrationof H202 is reducedwhen sulfateaerosolsareformed dueto the reactionof SO2+ H202in clouddroplets.The gas-phasereactionSO: + OH convertsOH to HO2,but the reduction of OH andenhancementof HO2are insignificant( 3%). (2) The heterogeneousreactionof HO2 onthe surfaceof sulfateaerosolsproducesupto 10% reductio