Zeuch, Thomas

[["dc.bibliographiccitation.firstpage","15637"],["dc.bibliographiccitation.issue","45"],["dc.bibliographiccitation.journal","Physical Chemistry Chemical Physics"],["dc.bibliographiccitation.lastpage","15640"],["dc.bibliographiccitation.volume","14"],["dc.contributor.author","Carlsson, Philip Thomas Michael"],["dc.contributor.author","Keunecke, Claudia"],["dc.contributor.author","Krueger, Bastian Christopher"],["dc.contributor.author","Maass, Mona C."],["dc.contributor.author","Zeuch, Thomas"],["dc.date.accessioned","2018-11-07T09:14:50Z"],["dc.date.available","2018-11-07T09:14:50Z"],["dc.date.issued","2012"],["dc.description.abstract","Recent studies have suggested that the reaction of stabilised Criegee Intermediates (CIs) with sulfur dioxide (SO2), leading to the formation of a carbonyl compound and sulfur trioxide, is a relevant atmospheric source of sulfuric acid. Here, the significance of this pathway has been examined by studying the formation of gas phase products and aerosol during the ozonolysis of beta-pinene and 2-butene in the presence of SO2 in the pressure range of 10 to 1000 mbar. For b-pinene at atmospheric pressure, the addition of SO2 suppresses the formation of the secondary ozonide and leads to highly increased nopinone yields. A complete consumption of SO2 is observed at initial SO2 concentrations below the yield of stabilised CIs. In experiments using 2-butene a significant consumption of SO2 and additional formation of acetaldehyde are observed at 1 bar. A consistent kinetic simulation of the experimental findings is possible when a fast CI + SO2 reaction rate in the range of recent direct measurements [Welz et al., Science, 2012, 335, 204] is used. For 2-butene the addition of SO2 drastically increases the observed aerosol yields at higher pressures. Below 60 mbar the SO2 oxidation induced particle formation becomes inefficient pointing to the critical role of collisional stabilisation for sulfuric acid controlled nucleation at low pressures."],["dc.description.sponsorship","DFG [GRK 782]"],["dc.identifier.doi","10.1039/c2cp42992f"],["dc.identifier.isi","000310460400002"],["dc.identifier.pmid","23090096"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/10222"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/27518"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Royal Soc Chemistry"],["dc.relation.issn","1463-9084"],["dc.relation.issn","1463-9076"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","Sulfur dioxide oxidation induced mechanistic branching and particle formation during the ozonolysis of beta-pinene and 2-butene"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","715"],["dc.bibliographiccitation.issue","3"],["dc.bibliographiccitation.journal","Angewandte Chemie International Edition"],["dc.bibliographiccitation.lastpage","719"],["dc.bibliographiccitation.volume","53"],["dc.contributor.author","Ahrens, Jennifer"],["dc.contributor.author","Carlsson, Philip Thomas Michael"],["dc.contributor.author","Hertl, Nils"],["dc.contributor.author","Olzmann, Matthias"],["dc.contributor.author","Pfeifle, Mark"],["dc.contributor.author","Wolf, Jan Lennard"],["dc.contributor.author","Zeuch, Thomas"],["dc.date.accessioned","2018-11-07T09:45:09Z"],["dc.date.available","2018-11-07T09:45:09Z"],["dc.date.issued","2014"],["dc.description.abstract","Recently, direct kinetic experiments have shown that the oxidation of sulfur dioxide to sulfur trioxide by reaction with stabilized Criegee intermediates (CIs) is an important source of sulfuric acid in the atmosphere. So far, only small CIs, generated in photolysis experiments, have been directly detected. Herein, it is shown that large, stabilized CIs can be detected in the gas phase by FTIR spectroscopy during the ozonolysis of beta-pinene. Their transient absorption bands between 930 and 830 cm(-1) appear only in the initial phase of the ozonolysis reaction when the scavenging of stabilized CIs by the reaction products is slow. The large CIs react with sulfur dioxide to give sulfur trioxide and nopinone with a yield exceeding 80%. Reactant consumption and product formation in time-resolved beta-pinene ozonolysis experiments in the presence of sulfur dioxide have been kinetically modeled. The results suggest a fast reaction of sulfur dioxide with CIs arising from b-pinene ozonolysis."],["dc.description.sponsorship","DFG [GRK 782]"],["dc.identifier.doi","10.1002/anie.201307327"],["dc.identifier.isi","000330983300010"],["dc.identifier.pmid","24402798"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/34554"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Wiley-v C H Verlag Gmbh"],["dc.relation.issn","1521-3773"],["dc.relation.issn","1433-7851"],["dc.title","Infrared Detection of Criegee Intermediates Formed during the Ozonolysis of beta-Pinene and Their Reactivity towards Sulfur Dioxide"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","11695"],["dc.bibliographiccitation.issue","33"],["dc.bibliographiccitation.journal","Physical Chemistry Chemical Physics"],["dc.bibliographiccitation.lastpage","11705"],["dc.bibliographiccitation.volume","14"],["dc.contributor.author","Carlsson, Philip Thomas Michael"],["dc.contributor.author","Dege, Janina Elisabeth"],["dc.contributor.author","Keunecke, Claudia"],["dc.contributor.author","Krueger, Bastian Christopher"],["dc.contributor.author","Wolf, Jan Lennard"],["dc.contributor.author","Zeuch, Thomas"],["dc.date.accessioned","2018-11-07T09:15:06Z"],["dc.date.available","2018-11-07T09:15:06Z"],["dc.date.issued","2012"],["dc.description.abstract","The ozonolysis of cyclohexene is studied with respect to the pressure dependent formation of stable gas-phase products and secondary organic aerosol (SOA) as well as the influence of the presence of SO2. In addition the rate coefficient for the initial reaction cyclohexene + O-3 was determined at 295 K. The observed increase in CO and ethene yields at low pressures and the absence of ketene in the product spectrum confirm previously proposed reaction pathways forming these decomposition products. An enhanced ethene formation at pressures below 300 mbar coincides with drastically decreased aerosol yields pointing to a high influence on SOA formation of chemical activation driven dynamics in the vinylhydroperoxide channel. The static reactor experiments at 450 mbar in the presence of SO2 in the present study showed a similar sensitivity of additional particle formation to H2SO4 number densities as found in near-atmospheric flow reactor experiments [Sipila et al., Science, 2010, 327, 1243], a surprising result with regard to the very different experimental approaches. At low pressures (around 40 mbar) no significant new particle formation is observed even at high H2SO4 concentrations. These findings indicate that the collisional stabilisation of initial clusters is an important aspect for SOA formation processes involving sulfuric acid and organic compounds. The results may have implications for geo-engineering strategies based on stratospheric sulfur injection, but caution is mandatory when room temperature laboratory results are extrapolated to stratospheric conditions."],["dc.description.sponsorship","DFG [GRK 782]; Fonds der Chemischen Industrie"],["dc.identifier.doi","10.1039/c2cp40714k"],["dc.identifier.isi","000307017800015"],["dc.identifier.pmid","22825796"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/10230"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/27593"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Royal Soc Chemistry"],["dc.relation.issn","1463-9076"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","Pressure dependent aerosol formation from the cyclohexene gas-phase ozonolysis in the presence and absence of sulfur dioxide: a new perspective on the stabilisation of the initial clusters"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]