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Titel |
Experimental and theoretical studies on the OH-initiated degradation of tert-butylamine |
VerfasserIn |
Wen Tan, Barbara D'Anna, Philipp Eichler, Tomas Mikoviny, Markus Müller, Claus Jørgen Nielsen, Armin Wisthaler, Liang Zhu |
Konferenz |
EGU General Assembly 2017
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Medientyp |
Artikel
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Sprache |
en
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Digitales Dokument |
PDF |
Erschienen |
In: GRA - Volume 19 (2017) |
Datensatznummer |
250143544
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Publikation (Nr.) |
EGU/EGU2017-7275.pdf |
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Zusammenfassung |
Amine-based carbon dioxide (CO2) capture facilities release small amounts of amines into
the atmosphere. Once airborne, the amines are photochemically transformed into
imines, amides, nitrosamines, nitramines and other breakdown products. As some of
these products pose a risk to human health and the environment, we have elucidated
photochemical decomposition mechanisms of various types of amines in previous work.
Our studies did, however, not include amines in which the primary amino group
is attached to a tertiary carbon atom, with 2-amino-2-methyl-1-propanol (AMP,
(CH3)2C(NH2)CH2OH) being a prominent candidate used in CO2 capture. Our initial step in
elucidating the degradation mechanism of AMP was to study tert-butylamine (tBA,
(CH3)3C(NH2)), which is a similar molecule but lacks the OH group. OH-initiated
degradation of tBA was studied in chamber experiments at the European Photoreactor
(EUPHORE) in Valencia (Spain) using state-of-the-art analytical instrumentation. A
Proton-Transfer-Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS) was used to
measure tBA and tBA degradation products in the gas phase. Propan-2-imine (PI,
(CH3)2C(=NH)) and tert-butylnitramine (tBNA, (CH3)3C(NHNO2)) were observed as
the two major gas-phase products. An Aerosol Mass Spectrometer (AMS) made
quantitative measurements of tert-butylaminium nitrate in the particle phase. A
PTR-ToF-MS instrument equipped with a “chemical analysis of aerosol online” (CHARON)
inlet detected the two major tBA degradation products (PI, tBNA) in the particle
phase. Experimental work was supplemented by quantum chemistry calculations.
We will present measured product yields and a complete degradation scheme of
tBA.
This work was supported by the Norwegian Research Council CLIMIT program under
contract 244055. |
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