000840312 001__ 840312
000840312 005__ 20240712101004.0
000840312 0247_ $$2doi$$a10.1039/C7CP05541B
000840312 0247_ $$2ISSN$$a1463-9076
000840312 0247_ $$2ISSN$$a1463-9084
000840312 0247_ $$2Handle$$a2128/16555
000840312 0247_ $$2pmid$$apmid:29182168
000840312 0247_ $$2WOS$$aWOS:000417295800009
000840312 037__ $$aFZJ-2017-07854
000840312 041__ $$aEnglish
000840312 082__ $$a540
000840312 1001_ $$0P:(DE-Juel1)167140$$aVereecken, L.$$b0$$eCorresponding author
000840312 245__ $$aUnimolecular decay strongly limits the atmospheric impact of Criegee intermediates
000840312 260__ $$aCambridge$$bRSC Publ.$$c2017
000840312 3367_ $$2DRIVER$$aarticle
000840312 3367_ $$2DataCite$$aOutput Types/Journal article
000840312 3367_ $$0PUB:(DE-HGF)16$$2PUB:(DE-HGF)$$aJournal Article$$bjournal$$mjournal$$s1552644432_21967
000840312 3367_ $$2BibTeX$$aARTICLE
000840312 3367_ $$2ORCID$$aJOURNAL_ARTICLE
000840312 3367_ $$00$$2EndNote$$aJournal Article
000840312 520__ $$aStabilized Criegee intermediates (SCI) are reactive oxygenated species formed in the ozonolysis of hydrocarbons. Their chemistry could influence the oxidative capacity of the atmosphere by affecting the HOx and NOx cycles, or by the formation of low-volatility oxygenates enhancing atmospheric aerosols known to have an important impact on climate. The concentration of SCI in the atmosphere has hitherto not been determined reliably, and very little is known about their speciation. Here we show that the concentration of biogenic SCI is strongly limited by their unimolecular decay, based on extensive theory-based structure–activity relationships (SARs) for the reaction rates for decomposition. Reaction with water vapor, H2O and (H2O)2 molecules, is the second most important loss process; SARs are also proposed for these reactions. For SCI derived from the most common biogenic VOCs, we find that unimolecular decay is responsible for just over half of the loss, with reaction with water vapor the main remaining loss process. Reactions with SO2, NO2, or acids have negligible impact on the atmospheric SCI concentration. The ambient SCI concentrations are further characterized by analysis of field data with speciated hydrocarbon information, and by implementation of the chemistry in a global chemistry model. The results show a highly complex SCI speciation, with an atmospheric peak SCI concentrations below 1 × 105 molecule cm−3, and annual average SCI concentrations less than 7 × 103 molecule cm−3. We find that SCI have only a negligible impact on the global gas phase H2SO4 formation or removal of oxygenates, though some contribution around the equatorial belt, and in select regions, cannot be excluded.
000840312 536__ $$0G:(DE-HGF)POF3-243$$a243 - Tropospheric trace substances and their transformation processes (POF3-243)$$cPOF3-243$$fPOF III$$x0
000840312 536__ $$0G:(DE-Juel1)jicg23_20151101$$aChemical processes in the troposphere and their impact on climate (jicg23_20151101)$$cjicg23_20151101$$fChemical processes in the troposphere and their impact on climate$$x1
000840312 588__ $$aDataset connected to CrossRef
000840312 65027 $$0V:(DE-MLZ)SciArea-110$$2V:(DE-HGF)$$aChemistry$$x0
000840312 7001_ $$0P:(DE-Juel1)166537$$aNovelli, A.$$b1
000840312 7001_ $$0P:(DE-Juel1)167439$$aTaraborrelli, D.$$b2
000840312 773__ $$0PERI:(DE-600)1476244-4$$a10.1039/C7CP05541B$$gp. 10.1039.C7CP05541B$$n19$$p31599--31612$$tPhysical chemistry, chemical physics$$v47$$x1463-9084$$y2017
000840312 8564_ $$uhttps://juser.fz-juelich.de/record/840312/files/c7cp05541b-1.pdf$$yOpenAccess
000840312 8564_ $$uhttps://juser.fz-juelich.de/record/840312/files/c7cp05541b-1.gif?subformat=icon$$xicon$$yOpenAccess
000840312 8564_ $$uhttps://juser.fz-juelich.de/record/840312/files/c7cp05541b-1.jpg?subformat=icon-1440$$xicon-1440$$yOpenAccess
000840312 8564_ $$uhttps://juser.fz-juelich.de/record/840312/files/c7cp05541b-1.jpg?subformat=icon-180$$xicon-180$$yOpenAccess
000840312 8564_ $$uhttps://juser.fz-juelich.de/record/840312/files/c7cp05541b-1.jpg?subformat=icon-640$$xicon-640$$yOpenAccess
000840312 8564_ $$uhttps://juser.fz-juelich.de/record/840312/files/c7cp05541b-1.pdf?subformat=pdfa$$xpdfa$$yOpenAccess
000840312 8767_ $$8SL26551$$92017-10-25$$d2017-10-25$$eHybrid-OA$$jZahlung erfolgt$$pCP-ART-08-2017-005541.R1$$zGBP 1600,-
000840312 909CO $$ooai:juser.fz-juelich.de:840312$$pdnbdelivery$$popenCost$$pVDB$$pVDB:Earth_Environment$$pdriver$$pOpenAPC$$popen_access$$popenaire
000840312 9101_ $$0I:(DE-588b)5008462-8$$6P:(DE-Juel1)167140$$aForschungszentrum Jülich$$b0$$kFZJ
000840312 9101_ $$0I:(DE-588b)5008462-8$$6P:(DE-Juel1)166537$$aForschungszentrum Jülich$$b1$$kFZJ
000840312 9101_ $$0I:(DE-588b)5008462-8$$6P:(DE-Juel1)167439$$aForschungszentrum Jülich$$b2$$kFZJ
000840312 9131_ $$0G:(DE-HGF)POF3-243$$1G:(DE-HGF)POF3-240$$2G:(DE-HGF)POF3-200$$3G:(DE-HGF)POF3$$4G:(DE-HGF)POF$$aDE-HGF$$bErde und Umwelt$$lAtmosphäre und Klima$$vTropospheric trace substances and their transformation processes$$x0
000840312 9141_ $$y2017
000840312 915__ $$0LIC:(DE-HGF)CCBY3$$2HGFVOC$$aCreative Commons Attribution CC BY 3.0
000840312 915__ $$0StatID:(DE-HGF)0200$$2StatID$$aDBCoverage$$bSCOPUS
000840312 915__ $$0StatID:(DE-HGF)0510$$2StatID$$aOpenAccess
000840312 915__ $$0StatID:(DE-HGF)0100$$2StatID$$aJCR$$bPHYS CHEM CHEM PHYS : 2015
000840312 915__ $$0StatID:(DE-HGF)0150$$2StatID$$aDBCoverage$$bWeb of Science Core Collection
000840312 915__ $$0StatID:(DE-HGF)0110$$2StatID$$aWoS$$bScience Citation Index
000840312 915__ $$0StatID:(DE-HGF)0111$$2StatID$$aWoS$$bScience Citation Index Expanded
000840312 915__ $$0StatID:(DE-HGF)9900$$2StatID$$aIF < 5
000840312 915__ $$0StatID:(DE-HGF)0400$$2StatID$$aAllianz-Lizenz / DFG
000840312 915__ $$0StatID:(DE-HGF)1150$$2StatID$$aDBCoverage$$bCurrent Contents - Physical, Chemical and Earth Sciences
000840312 915__ $$0StatID:(DE-HGF)0310$$2StatID$$aDBCoverage$$bNCBI Molecular Biology Database
000840312 915__ $$0StatID:(DE-HGF)0300$$2StatID$$aDBCoverage$$bMedline
000840312 915__ $$0StatID:(DE-HGF)0420$$2StatID$$aNationallizenz
000840312 915__ $$0StatID:(DE-HGF)0199$$2StatID$$aDBCoverage$$bThomson Reuters Master Journal List
000840312 920__ $$lyes
000840312 9201_ $$0I:(DE-Juel1)IEK-8-20101013$$kIEK-8$$lTroposphäre$$x0
000840312 9201_ $$0I:(DE-82)080012_20140620$$kJARA-HPC$$lJARA - HPC$$x1
000840312 9801_ $$aAPC
000840312 9801_ $$aFullTexts
000840312 980__ $$ajournal
000840312 980__ $$aVDB
000840312 980__ $$aI:(DE-Juel1)IEK-8-20101013
000840312 980__ $$aI:(DE-82)080012_20140620
000840312 980__ $$aAPC
000840312 980__ $$aUNRESTRICTED
000840312 981__ $$aI:(DE-Juel1)ICE-3-20101013