Publikation:
A parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models

Kurzanzeige
dc.contributor.authorChen, Ying-Yuan
dc.contributor.authorBirmili, Wolfram
dc.contributor.authorWolke, Ralf
dc.contributor.authorRan, Liang
dc.date.accessioned2024-06-16T15:24:32Z
dc.date.available2024-06-16T15:24:32Z
dc.date.issued2018
dc.description.abstractThe heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R?=??0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMOŃMUSCAT, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10Ń25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5Ń19, with the corrected NH3 emissions (reduced by 50?%) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ?~??35?%. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17Ń18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2?% on average and 20?% at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe. Quelle: https://www.atmos-chem-phys.net/en
dc.format.extent1 Onlineressource (Seite 673-689)
dc.format.mediumonline resource
dc.identifier.doihttps://doi.org/10.60810/openumwelt-1600
dc.identifier.urihttps://openumwelt.de/handle/123456789/6406
dc.language.isoeng
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/
dc.titleA parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models
dc.typeWissenschaftlicher Artikel
dc.type.dcmitext
dc.type.mediumcomputer
dspace.entity.typePublication
local.bibliographicCitation.journalTitleAtmospheric Chemistry & Physics
local.bibliographicCitation.originalDOI10.5194/acp-18-673-2018
local.bibliographicCitation.volume18 (2018), Heft 2
local.collectionAufsätze
local.contributor.authorId00313942
local.contributor.authorId00348700
local.contributor.authorId02174687
local.identifier.catalogId02452742
local.ingest.leader06620naa a2200000uu 4500
local.jointTitleA PARAMETERIZATION OF THE HETEROGENEOUS HYDROLYSIS OF N2O5 FOR MASSBASED AEROSOL MODELS IMPROVEMENT OF PARTICULATE NITRATE PREDICTION
local.reviewtrue
local.sourcecatalog
local.source.urihttp://webde/gruppen/bibliothek/Einzelaufsaetze/Einzelaufsaetze-EA/EA005347.pdf
local.staffPublicationtrue
local.subtitleimprovement of particulate nitrate prediction
relation.isAuthorOfPublication530a7f84-0626-465c-8eb4-c1bb5e4b1ca6
relation.isAuthorOfPublication.latestForDiscovery530a7f84-0626-465c-8eb4-c1bb5e4b1ca6
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