Chemistry and Photochemistry of Pyruvic Acid at the Air-Water Interface
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Chemistry and Photochemistry of Pyruvic Acid at the Air-Water Interface. / Kappes, Keaten J.; Deal, Alexandra M.; Jespersen, Malte F.; Blair, Sandra L.; Doussin, Jean Francois; Cazaunau, Mathieu; Pangui, Edouard; Hopper, Brianna N.; Johnson, Matthew S.; Vaida, Veronica.
I: Journal of Physical Chemistry A, Bind 125, Nr. 4, 04.02.2021, s. 1036-1049.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Chemistry and Photochemistry of Pyruvic Acid at the Air-Water Interface
AU - Kappes, Keaten J.
AU - Deal, Alexandra M.
AU - Jespersen, Malte F.
AU - Blair, Sandra L.
AU - Doussin, Jean Francois
AU - Cazaunau, Mathieu
AU - Pangui, Edouard
AU - Hopper, Brianna N.
AU - Johnson, Matthew S.
AU - Vaida, Veronica
PY - 2021/2/4
Y1 - 2021/2/4
N2 - Interfacial regions are unique chemical reaction environments that can promote chemistry not found elsewhere. The air-water interface is ubiquitous in the natural environment in the form of ocean surfaces and aqueous atmospheric aerosols. Here we investigate the chemistry and photochemistry of pyruvic acid (PA), a common environmental species, at the air-water interface and compare it to its aqueous bulk chemistry using two different experimental setups: (1) a Langmuir-Blodgett trough, which models natural water surfaces and provides a direct comparison between the two reaction environments, and (2) an atmospheric simulation chamber (CESAM) to monitor the chemical processing of nebulized aqueous PA droplets. The results show that surface chemistry leads to substantial oligomer formation. The sequence begins with the condensation of lactic acid (LA), formed at the surface, with itself and with pyruvic acid, and LA + LA - H2O and LA + PA - H2O are prominent among the products in addition to a series of higher-molecular-weight oligomers of mixed units of PA and LA. In addition, we see zymonic acid at the surface. Actinic radiation enhances the production of the oligomers and produces additional surface-active molecules known from the established aqueous photochemical mechanisms. The presence and formation of complex organic molecules at the air-water interface from a simple precursor like PA in the natural environment is relevant to contemporary atmospheric science and is important in the context of prebiotic chemistry, where abiotic production of complex molecules is necessary for abiogenesis.
AB - Interfacial regions are unique chemical reaction environments that can promote chemistry not found elsewhere. The air-water interface is ubiquitous in the natural environment in the form of ocean surfaces and aqueous atmospheric aerosols. Here we investigate the chemistry and photochemistry of pyruvic acid (PA), a common environmental species, at the air-water interface and compare it to its aqueous bulk chemistry using two different experimental setups: (1) a Langmuir-Blodgett trough, which models natural water surfaces and provides a direct comparison between the two reaction environments, and (2) an atmospheric simulation chamber (CESAM) to monitor the chemical processing of nebulized aqueous PA droplets. The results show that surface chemistry leads to substantial oligomer formation. The sequence begins with the condensation of lactic acid (LA), formed at the surface, with itself and with pyruvic acid, and LA + LA - H2O and LA + PA - H2O are prominent among the products in addition to a series of higher-molecular-weight oligomers of mixed units of PA and LA. In addition, we see zymonic acid at the surface. Actinic radiation enhances the production of the oligomers and produces additional surface-active molecules known from the established aqueous photochemical mechanisms. The presence and formation of complex organic molecules at the air-water interface from a simple precursor like PA in the natural environment is relevant to contemporary atmospheric science and is important in the context of prebiotic chemistry, where abiotic production of complex molecules is necessary for abiogenesis.
U2 - 10.1021/acs.jpca.0c09096
DO - 10.1021/acs.jpca.0c09096
M3 - Journal article
C2 - 33475373
AN - SCOPUS:85100423615
VL - 125
SP - 1036
EP - 1049
JO - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory
JF - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory
SN - 1089-5639
IS - 4
ER -
ID: 260947111