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Theoretical and Experimental Study on the Reaction of tert-Butylamine with OH Radicals in the Atmosphere

Artikel i vetenskaplig tidskrift
Författare Wen Tan
Liang Zhu
Tomáš Mikoviny
Claus J. Nielsen
Armin Wisthaler
Philipp Eichler
Markus Müller
Barbara D'Anna
Naomi J. Farren
Jacqueline F. Hamilton
Jan B. C. Pettersson
Mattias Hallquist
Simen Antonsen
Yngve Stenstrøm
Publicerad i Journal of Physical Chemistry A
Volym 122
Nummer/häfte 18
Sidor 4470-4480
ISSN 10895639
Publiceringsår 2018
Publicerad vid Institutionen för kemi och molekylärbiologi
Sidor 4470-4480
Språk en
Länkar https://doi.org/10.1021/acs.jpca.8b...
Ämneskategorier Kemi, Analytisk kemi, Fysikalisk kemi, Klimatforskning, Miljövetenskap, Miljökemi, Meteorologi och atmosfärforskning, Organisk kemi

Sammanfattning

© 2018 American Chemical Society. The OH-initiated atmospheric degradation of tert-butylamine (tBA), (CH 3 ) 3 CNH 2 , was investigated in a detailed quantum chemistry study and in laboratory experiments at the European Photoreactor (EUPHORE) in Spain. The reaction was found to mainly proceed via hydrogen abstraction from the amino group, which in the presence of nitrogen oxides (NO x ), generates tert-butylnitramine, (CH 3 ) 3 CNHNO 2 , and acetone as the main reaction products. Acetone is formed via the reaction of tert-butylnitrosamine, (CH 3 ) 3 CNHNO, and/or its isomer tert-butylhydroxydiazene, (CH 3 ) 3 CN=NOH, with OH radicals, which yield nitrous oxide (N 2 O) and the (CH 3 ) 3 Ċ radical. The latter is converted to acetone and formaldehyde. Minor predicted and observed reaction products include formaldehyde, 2-methylpropene, acetamide and propan-2-imine. The reaction in the EUPHORE chamber was accompanied by strong particle formation which was induced by an acid-base reaction between photochemically formed nitric acid and the reagent amine. The tert-butylaminium nitrate salt was found to be of low volatility, with a vapor pressure of 5.1 × 10 -6 Pa at 298 K. The rate of reaction between tert-butylamine and OH radicals was measured to be 8.4 (±1.7) × 10 -12 cm 3 molecule -1 s -1 at 305 ± 2 K and 1015 ± 1 hPa.

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