Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation
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) m...
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Published in | Atmospheric measurement techniques Vol. 11; no. 8; pp. 4763 - 4773 |
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Main Authors | , , , , , |
Format | Journal Article |
Language | English |
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14.08.2018
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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. |
---|---|
AbstractList | 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 (C.sub.10 H.sub.17 .sup.+) and m/z = 81.070 (C.sub.6 H.sub.9 .sup.+) 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. 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. 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. 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. |
Audience | Academic |
Author | Fischer, Lukas Hansel, Armin Bernhammer, Anne-Kathrin Heinritzi, Martin Simon, Mario Mentler, Bernhard |
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ContentType | Journal Article |
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Snippet | During nucleation studies from pure isoprene oxidation in the CLOUD chamber
at the European Organization for Nuclear Research (CERN) we observed
unexpected ion... During nucleation studies from pure isoprene oxidation in the CLOUD chamber at the European Organization for Nuclear Research (CERN) we observed unexpected ion... |
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SubjectTerms | Analysis Association reactions Atmospheric conditions C5 hydrocarbons Cloud chambers Clouds Contaminants Cycloaddition Growth rate Ions Isoprene Limonene Mass spectrometry Monoterpenes Nuclear reactions Nuclear research Nucleation Organic chemistry Organizations Oxidation Oxidation-reduction reactions Oxygenation Ozonolysis Particle formation Properties Quality assurance Ratios Reaction time Terpenes Trace contaminants Volatility |
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Title | Production of highly oxygenated organic molecules (HOMs) from trace contaminants during isoprene oxidation |
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