dc.date.accessioned | 2021-04-07T18:57:52Z | |
dc.date.available | 2021-04-07T18:57:52Z | |
dc.date.created | 2020-12-30T20:21:27Z | |
dc.date.issued | 2021 | |
dc.identifier.citation | Tan, Wen Zhu, Liang Mikoviny, Tomas Nielsen, Claus Jørgen Wisthaler, Armin D´Anna, Barbara Antonsen, Simen Gjelseth Stenstrøm, Yngve H. Farren, Naomi J. Hamilton, Jacqueline F. Boustead, Graham A. . Experimental and Theoretical Study of the OH-Initiated Degradation of Piperazine under Simulated Atmospheric Conditions. Journal of Physical Chemistry A. 2020 | |
dc.identifier.uri | http://hdl.handle.net/10852/85073 | |
dc.description.abstract | The OH-initiated photo-oxidation of piperazine and 1-nitropiperazine as well as the photolysis of 1-nitrosopiperazine were investigated in a large atmospheric simulation chamber. The rate coefficient for the reaction of piperazine with OH radicals was determined by the relative rate method to be kOH-piperazine = (2.8 ± 0.6) × 10–10 cm3 molecule–1 s–1 at 307 ± 2 K and 1014 ± 2 hPa. Product studies showed the piperazine + OH reaction to proceed both via C–H and N–H abstraction, resulting in the formation of 1,2,3,6-tetrahydropyrazine as the major product and in 1-nitropiperazine and 1-nitrosopiperazine as minor products. The branching in the piperazinyl radical reactions with NO, NO2, and O2 was obtained from 1-nitrosopiperazine photolysis experiments and employed analyses of the 1-nitropiperazine and 1-nitrosopiperazine temporal profiles observed during piperazine photo-oxidation. The derived initial branching between N–H and C–H abstraction by OH radicals, kN–H/(kN–H + kC–H), was 0.18 ± 0.04. All experiments were accompanied by substantial aerosol formation that was initiated by the reaction of piperazine with nitric acid. Both primary and secondary photo-oxidation products including 1-nitropiperazine and 1,4-dinitropiperazine were detected in the aerosol particles formed. Corroborating atmospheric photo-oxidation schemes for piperazine and 1-nitropiperazine were derived from M06-2X/aug-cc-pVTZ quantum chemistry calculations and master equation modeling of the pivotal reaction steps. The atmospheric chemistry of piperazine is evaluated, and a validated chemical mechanism for implementation in dispersion models is presented. | |
dc.language | EN | |
dc.publisher | ACS Publications | |
dc.rights | Attribution 4.0 International | |
dc.rights.uri | https://creativecommons.org/licenses/by/4.0/ | |
dc.title | Experimental and Theoretical Study of the OH-Initiated Degradation of Piperazine under Simulated Atmospheric Conditions | |
dc.type | Journal article | |
dc.creator.author | Tan, Wen | |
dc.creator.author | Zhu, Liang | |
dc.creator.author | Mikoviny, Tomas | |
dc.creator.author | Nielsen, Claus Jørgen | |
dc.creator.author | Wisthaler, Armin | |
dc.creator.author | D´Anna, Barbara | |
dc.creator.author | Antonsen, Simen Gjelseth | |
dc.creator.author | Stenstrøm, Yngve H. | |
dc.creator.author | Farren, Naomi J. | |
dc.creator.author | Hamilton, Jacqueline F. | |
dc.creator.author | Boustead, Graham A. | |
cristin.unitcode | 185,15,12,0 | |
cristin.unitname | Kjemisk institutt | |
cristin.ispublished | true | |
cristin.fulltext | postprint | |
cristin.qualitycode | 1 | |
dc.identifier.cristin | 1864156 | |
dc.identifier.bibliographiccitation | info:ofi/fmt:kev:mtx:ctx&ctx_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.jtitle=Journal of Physical Chemistry A&rft.volume=&rft.spage=&rft.date=2020 | |
dc.identifier.jtitle | Journal of Physical Chemistry A | |
dc.identifier.volume | 125 | |
dc.identifier.issue | 1 | |
dc.identifier.startpage | 411 | |
dc.identifier.endpage | 422 | |
dc.identifier.doi | https://doi.org/10.1021/acs.jpca.0c10223 | |
dc.identifier.urn | URN:NBN:no-87795 | |
dc.type.document | Tidsskriftartikkel | |
dc.type.peerreviewed | Peer reviewed | |
dc.source.issn | 1089-5639 | |
dc.identifier.fulltext | Fulltext https://www.duo.uio.no/bitstream/handle/10852/85073/4/acs.jpca.0c10223.pdf | |
dc.type.version | PublishedVersion | |