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Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation
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Zeitschriftentitel: | Atmospheric Measurement Techniques |
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Personen und Körperschaften: | , , , , , |
In: | Atmospheric Measurement Techniques, 11, 2018, 8, S. 4763-4773 |
Format: | E-Article |
Sprache: | Englisch |
veröffentlicht: |
Copernicus GmbH
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author_facet |
Bernhammer, Anne-Kathrin Fischer, Lukas Mentler, Bernhard Heinritzi, Martin Simon, Mario Hansel, Armin Bernhammer, Anne-Kathrin Fischer, Lukas Mentler, Bernhard Heinritzi, Martin Simon, Mario Hansel, Armin |
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author |
Bernhammer, Anne-Kathrin Fischer, Lukas Mentler, Bernhard Heinritzi, Martin Simon, Mario Hansel, Armin |
spellingShingle |
Bernhammer, Anne-Kathrin Fischer, Lukas Mentler, Bernhard Heinritzi, Martin Simon, Mario Hansel, Armin Atmospheric Measurement Techniques Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation Atmospheric Science |
author_sort |
bernhammer, anne-kathrin |
spelling |
Bernhammer, Anne-Kathrin Fischer, Lukas Mentler, Bernhard Heinritzi, Martin Simon, Mario Hansel, Armin 1867-8548 Copernicus GmbH Atmospheric Science http://dx.doi.org/10.5194/amt-11-4763-2018 <jats:p>Abstract. During nucleation studies from pure isoprene oxidation in the CLOUD chamber at the European Organization for Nuclear Research (CERN) we observed unexpected ion signals at m∕z = 137.133 (C10H17+) and m∕z = 81.070 (C6H9+) with the recently developed proton-transfer-reaction time-of-flight (PTR3-TOF) mass spectrometer instrument. The mass-to-charge ratios of these ion signals typically correspond to protonated monoterpenes and their main fragment. We identified two origins of these signals: first secondary association reactions of protonated isoprene with isoprene within the PTR3-TOF reaction chamber and secondly [4+2] cycloaddition (Diels–Alder) of isoprene inside the gas bottle which presumably forms the favored monoterpenes limonene and sylvestrene, as known from literature. Under our PTR3-TOF conditions used in 2016 an amount (relative to isoprene) of 2 % is formed within the PTR3-TOF reaction chamber and 1 % is already present in the gas bottle. The presence of unwanted cycloaddition products in the CLOUD chamber impacts the nucleation studies by creating ozonolysis products as the corresponding monoterpenes and is responsible for the majority of the observed highly oxygenated organic molecules (HOMs), which in turn leads to a significant overestimation of both the nucleation rate and the growth rate. In order to study new particle formation (NPF) from pure isoprene oxidation under relevant atmospheric conditions, it is important to improve and assure the quality and purity of the precursor isoprene. This was successfully achieved by cryogenically trapping lower-volatility compounds such as monoterpenes before isoprene was introduced into the CLOUD chamber. </jats:p> Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation Atmospheric Measurement Techniques |
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10.5194/amt-11-4763-2018 |
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title |
Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_unstemmed |
Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_full |
Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_fullStr |
Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_full_unstemmed |
Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_short |
Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_sort |
production of highly oxygenated organic molecules (homs) from trace contaminants during isoprene oxidation |
topic |
Atmospheric Science |
url |
http://dx.doi.org/10.5194/amt-11-4763-2018 |
publishDate |
2018 |
physical |
4763-4773 |
description |
<jats:p>Abstract. During nucleation studies from pure isoprene oxidation in the CLOUD chamber
at the European Organization for Nuclear Research (CERN) we observed
unexpected ion signals at m∕z = 137.133
(C10H17+) and m∕z = 81.070
(C6H9+) with the recently developed
proton-transfer-reaction time-of-flight (PTR3-TOF) mass spectrometer
instrument. The mass-to-charge ratios of these ion signals typically
correspond to protonated monoterpenes and their main fragment. We identified
two origins of these signals: first secondary association reactions of
protonated isoprene with isoprene within the PTR3-TOF reaction chamber and
secondly [4+2] cycloaddition (Diels–Alder) of isoprene inside the gas
bottle which presumably forms the favored monoterpenes limonene and
sylvestrene, as known from literature. Under our PTR3-TOF conditions used in
2016 an amount (relative to isoprene) of 2 % is formed within the
PTR3-TOF reaction chamber and 1 % is already present in the gas bottle.
The presence of unwanted cycloaddition products in the CLOUD chamber impacts
the nucleation studies by creating ozonolysis products as the corresponding
monoterpenes and is responsible for the majority of the observed highly
oxygenated organic molecules (HOMs), which in turn leads to a significant
overestimation of both the nucleation rate and the growth rate. In order to
study new particle formation (NPF) from pure isoprene oxidation under
relevant atmospheric conditions, it is important to improve and assure the
quality and purity of the precursor isoprene. This was successfully achieved
by cryogenically trapping lower-volatility compounds such as monoterpenes
before isoprene was introduced into the CLOUD chamber.
</jats:p> |
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author | Bernhammer, Anne-Kathrin, Fischer, Lukas, Mentler, Bernhard, Heinritzi, Martin, Simon, Mario, Hansel, Armin |
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description | <jats:p>Abstract. During nucleation studies from pure isoprene oxidation in the CLOUD chamber at the European Organization for Nuclear Research (CERN) we observed unexpected ion signals at m∕z = 137.133 (C10H17+) and m∕z = 81.070 (C6H9+) with the recently developed proton-transfer-reaction time-of-flight (PTR3-TOF) mass spectrometer instrument. The mass-to-charge ratios of these ion signals typically correspond to protonated monoterpenes and their main fragment. We identified two origins of these signals: first secondary association reactions of protonated isoprene with isoprene within the PTR3-TOF reaction chamber and secondly [4+2] cycloaddition (Diels–Alder) of isoprene inside the gas bottle which presumably forms the favored monoterpenes limonene and sylvestrene, as known from literature. Under our PTR3-TOF conditions used in 2016 an amount (relative to isoprene) of 2 % is formed within the PTR3-TOF reaction chamber and 1 % is already present in the gas bottle. The presence of unwanted cycloaddition products in the CLOUD chamber impacts the nucleation studies by creating ozonolysis products as the corresponding monoterpenes and is responsible for the majority of the observed highly oxygenated organic molecules (HOMs), which in turn leads to a significant overestimation of both the nucleation rate and the growth rate. In order to study new particle formation (NPF) from pure isoprene oxidation under relevant atmospheric conditions, it is important to improve and assure the quality and purity of the precursor isoprene. This was successfully achieved by cryogenically trapping lower-volatility compounds such as monoterpenes before isoprene was introduced into the CLOUD chamber. </jats:p> |
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spelling | Bernhammer, Anne-Kathrin Fischer, Lukas Mentler, Bernhard Heinritzi, Martin Simon, Mario Hansel, Armin 1867-8548 Copernicus GmbH Atmospheric Science http://dx.doi.org/10.5194/amt-11-4763-2018 <jats:p>Abstract. During nucleation studies from pure isoprene oxidation in the CLOUD chamber at the European Organization for Nuclear Research (CERN) we observed unexpected ion signals at m∕z = 137.133 (C10H17+) and m∕z = 81.070 (C6H9+) with the recently developed proton-transfer-reaction time-of-flight (PTR3-TOF) mass spectrometer instrument. The mass-to-charge ratios of these ion signals typically correspond to protonated monoterpenes and their main fragment. We identified two origins of these signals: first secondary association reactions of protonated isoprene with isoprene within the PTR3-TOF reaction chamber and secondly [4+2] cycloaddition (Diels–Alder) of isoprene inside the gas bottle which presumably forms the favored monoterpenes limonene and sylvestrene, as known from literature. Under our PTR3-TOF conditions used in 2016 an amount (relative to isoprene) of 2 % is formed within the PTR3-TOF reaction chamber and 1 % is already present in the gas bottle. The presence of unwanted cycloaddition products in the CLOUD chamber impacts the nucleation studies by creating ozonolysis products as the corresponding monoterpenes and is responsible for the majority of the observed highly oxygenated organic molecules (HOMs), which in turn leads to a significant overestimation of both the nucleation rate and the growth rate. In order to study new particle formation (NPF) from pure isoprene oxidation under relevant atmospheric conditions, it is important to improve and assure the quality and purity of the precursor isoprene. This was successfully achieved by cryogenically trapping lower-volatility compounds such as monoterpenes before isoprene was introduced into the CLOUD chamber. </jats:p> Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation Atmospheric Measurement Techniques |
spellingShingle | Bernhammer, Anne-Kathrin, Fischer, Lukas, Mentler, Bernhard, Heinritzi, Martin, Simon, Mario, Hansel, Armin, Atmospheric Measurement Techniques, Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation, Atmospheric Science |
title | Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_full | Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_fullStr | Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_full_unstemmed | Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_short | Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
title_sort | production of highly oxygenated organic molecules (homs) from trace contaminants during isoprene oxidation |
title_unstemmed | Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
topic | Atmospheric Science |
url | http://dx.doi.org/10.5194/amt-11-4763-2018 |