Volatile organic compounds (VOCs) in photochemically aged air from the eastern and western Mediterranean

Hdl Handle:
http://hdl.handle.net/10034/620593
Title:
Volatile organic compounds (VOCs) in photochemically aged air from the eastern and western Mediterranean
Authors:
Derstroff, Bettina; Hueser, Imke; Bourtsoukidis, Efstratios; Crowley, John N.; Fischer, Horst; Gromov, Sergey; Harder, Hartwig; Janssen, Ruud; Kesselmeier, Juergen; Lelieveld, Jos; Mallik, Chinmay; Martinez, Monica; Novelli, Anna; Parchatka, Uwe; Phillips, Gavin J. ( 0000-0003-4443-0822 ) ; Sander, Rolf; Sauvage, Carina; Schuladen, Jan; Stoenner, Christof; Tomsche, Laura; Williams, Jonathan
Abstract:
During the summertime CYPHEX campaign (CYprus PHotochemical EXperiment 2014) in the eastern Mediterranean, multiple volatile organic compounds (VOCs) were measured from a 650 m hilltop site in western Cyprus (34° 57′ N/32° 23′ E). Periodic shifts in the northerly Etesian winds resulted in the site being alternately impacted by photochemically processed emissions from western (Spain, France, Italy) and eastern (Turkey, Greece) Europe. Furthermore, the site was situated within the residual layer/free troposphere during some nights which were characterized by high ozone and low relative humidity levels. In this study we examine the temporal variation of VOCs at the site. The sparse Mediterranean scrub vegetation generated diel cycles in the reactive biogenic hydrocarbon isoprene, from very low values at night to a diurnal median level of 80–100 pptv. In contrast, the oxygenated volatile organic compounds (OVOCs) methanol and acetone exhibited weak diel cycles and were approximately an order of magnitude higher in mixing ratio (ca. 2.5–3 ppbv median level by day, range: ca. 1–8 ppbv) than the locally emitted isoprene and aromatic compounds such as benzene and toluene. Acetic acid was present at mixing ratios between 0.05 and 4 ppbv with a median level of ca. 1.2 ppbv during the daytime. When data points directly affected by the residual layer/free troposphere were excluded, the acid followed a pronounced diel cycle, which was influenced by various local effects including photochemical production and loss, direct emission, dry deposition and scavenging from advecting air in fog banks. The Lagrangian model FLEXPART was used to determine transport patterns and photochemical processing times (between 12 h and several days) of air masses originating from eastern and western Europe. Ozone and many OVOC levels were  ∼  20 and  ∼  30–60 % higher, respectively, in air arriving from the east. Using the FLEXPART calculated transport time, the contribution of photochemical processing, sea surface contact and dilution was estimated. Methanol and acetone decreased with residence time in the marine boundary layer (MBL) with loss rate constants of 0.74 and 0.53 day−1 from eastern Europe and 0.70 and 0.34 day−1 from western Europe, respectively. Simulations using the EMAC model underestimate these loss rates. The missing sink in the calculation is most probably an oceanic uptake enhanced by microbial consumption of methanol and acetone, although the temporal and spatial variability in the source strength on the continents might play a role as well. Correlations between acetone and methanol were weaker in western air masses (r2  =  0.68), but were stronger in air masses measured after the shorter transport time from the east (r2  =  0.73).
Affiliation:
Max Planck Institute for Chemistry; Massachusetts Institute of Technology; Cyprus Institute; Forschungszentrum Juelich; University of Chester
Citation:
Derstroff, B., et. al. (2017). Volatile organic compounds (VOCs) in photochemically aged air from the eastern and western Mediterranean. Atmospheric Chemistry and Physics, 17, 9547-9566. DOI: 10.5194/acp-17-9547-2017
Publisher:
Copernicus Publications
Journal:
Atmospheric Chemistry and Physics
Publication Date:
9-Aug-2017
URI:
http://hdl.handle.net/10034/620593
DOI:
10.5194/acp-17-9547-2017
Additional Links:
https://www.atmos-chem-phys.net/17/9547/2017/acp-17-9547-2017.html
Type:
Article
Language:
en
EISSN:
1680-7324
Appears in Collections:
Natural Sciences

Full metadata record

DC FieldValue Language
dc.contributor.authorDerstroff, Bettinaen
dc.contributor.authorHueser, Imkeen
dc.contributor.authorBourtsoukidis, Efstratiosen
dc.contributor.authorCrowley, John N.en
dc.contributor.authorFischer, Horsten
dc.contributor.authorGromov, Sergeyen
dc.contributor.authorHarder, Hartwigen
dc.contributor.authorJanssen, Ruuden
dc.contributor.authorKesselmeier, Juergenen
dc.contributor.authorLelieveld, Josen
dc.contributor.authorMallik, Chinmayen
dc.contributor.authorMartinez, Monicaen
dc.contributor.authorNovelli, Annaen
dc.contributor.authorParchatka, Uween
dc.contributor.authorPhillips, Gavin J.en
dc.contributor.authorSander, Rolfen
dc.contributor.authorSauvage, Carinaen
dc.contributor.authorSchuladen, Janen
dc.contributor.authorStoenner, Christofen
dc.contributor.authorTomsche, Lauraen
dc.contributor.authorWilliams, Jonathanen
dc.date.accessioned2017-08-10T10:39:09Z-
dc.date.available2017-08-10T10:39:09Z-
dc.date.issued2017-08-09-
dc.identifier.citationDerstroff, B., et. al. (2017). Volatile organic compounds (VOCs) in photochemically aged air from the eastern and western Mediterranean. Atmospheric Chemistry and Physics, 17, 9547-9566. DOI: 10.5194/acp-17-9547-2017en
dc.identifier.doi10.5194/acp-17-9547-2017-
dc.identifier.urihttp://hdl.handle.net/10034/620593-
dc.description.abstractDuring the summertime CYPHEX campaign (CYprus PHotochemical EXperiment 2014) in the eastern Mediterranean, multiple volatile organic compounds (VOCs) were measured from a 650 m hilltop site in western Cyprus (34° 57′ N/32° 23′ E). Periodic shifts in the northerly Etesian winds resulted in the site being alternately impacted by photochemically processed emissions from western (Spain, France, Italy) and eastern (Turkey, Greece) Europe. Furthermore, the site was situated within the residual layer/free troposphere during some nights which were characterized by high ozone and low relative humidity levels. In this study we examine the temporal variation of VOCs at the site. The sparse Mediterranean scrub vegetation generated diel cycles in the reactive biogenic hydrocarbon isoprene, from very low values at night to a diurnal median level of 80–100 pptv. In contrast, the oxygenated volatile organic compounds (OVOCs) methanol and acetone exhibited weak diel cycles and were approximately an order of magnitude higher in mixing ratio (ca. 2.5–3 ppbv median level by day, range: ca. 1–8 ppbv) than the locally emitted isoprene and aromatic compounds such as benzene and toluene. Acetic acid was present at mixing ratios between 0.05 and 4 ppbv with a median level of ca. 1.2 ppbv during the daytime. When data points directly affected by the residual layer/free troposphere were excluded, the acid followed a pronounced diel cycle, which was influenced by various local effects including photochemical production and loss, direct emission, dry deposition and scavenging from advecting air in fog banks. The Lagrangian model FLEXPART was used to determine transport patterns and photochemical processing times (between 12 h and several days) of air masses originating from eastern and western Europe. Ozone and many OVOC levels were  ∼  20 and  ∼  30–60 % higher, respectively, in air arriving from the east. Using the FLEXPART calculated transport time, the contribution of photochemical processing, sea surface contact and dilution was estimated. Methanol and acetone decreased with residence time in the marine boundary layer (MBL) with loss rate constants of 0.74 and 0.53 day−1 from eastern Europe and 0.70 and 0.34 day−1 from western Europe, respectively. Simulations using the EMAC model underestimate these loss rates. The missing sink in the calculation is most probably an oceanic uptake enhanced by microbial consumption of methanol and acetone, although the temporal and spatial variability in the source strength on the continents might play a role as well. Correlations between acetone and methanol were weaker in western air masses (r2  =  0.68), but were stronger in air masses measured after the shorter transport time from the east (r2  =  0.73).en
dc.language.isoenen
dc.publisherCopernicus Publicationsen
dc.relation.urlhttps://www.atmos-chem-phys.net/17/9547/2017/acp-17-9547-2017.htmlen
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subjectAtmospheric chemistryen
dc.subjectEnvironmental chemistryen
dc.titleVolatile organic compounds (VOCs) in photochemically aged air from the eastern and western Mediterraneanen
dc.typeArticleen
dc.identifier.eissn1680-7324-
dc.contributor.departmentMax Planck Institute for Chemistry; Massachusetts Institute of Technology; Cyprus Institute; Forschungszentrum Juelich; University of Chesteren
dc.identifier.journalAtmospheric Chemistry and Physicsen
dc.date.accepted2017-06-29-
or.grant.openaccessYesen
rioxxterms.funderUnfundeden
rioxxterms.identifier.projectUnfundeden
rioxxterms.versionAMen
rioxxterms.licenseref.startdate2017-08-09-
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