By the same authors

From the same journal

Trends in stabilisation of Criegee intermediates from alkene ozonolysis

Research output: Contribution to journalArticlepeer-review

Standard

Trends in stabilisation of Criegee intermediates from alkene ozonolysis. / Newland, Mike; Nelson, Bethany; Muñoz, Amalia; Ródenas, Milagros; Vera, Teresa; Tárrega, Joan; Rickard, Andrew Robert.

In: Physical Chemistry Chemical Physics, Vol. 22, D0CP00897D, 04.06.2020, p. 13698-13706.

Research output: Contribution to journalArticlepeer-review

Harvard

Newland, M, Nelson, B, Muñoz, A, Ródenas, M, Vera, T, Tárrega, J & Rickard, AR 2020, 'Trends in stabilisation of Criegee intermediates from alkene ozonolysis', Physical Chemistry Chemical Physics, vol. 22, D0CP00897D, pp. 13698-13706. https://doi.org/10.1039/d0cp00897d

APA

Newland, M., Nelson, B., Muñoz, A., Ródenas, M., Vera, T., Tárrega, J., & Rickard, A. R. (2020). Trends in stabilisation of Criegee intermediates from alkene ozonolysis. Physical Chemistry Chemical Physics, 22, 13698-13706. [D0CP00897D]. https://doi.org/10.1039/d0cp00897d

Vancouver

Newland M, Nelson B, Muñoz A, Ródenas M, Vera T, Tárrega J et al. Trends in stabilisation of Criegee intermediates from alkene ozonolysis. Physical Chemistry Chemical Physics. 2020 Jun 4;22:13698-13706. D0CP00897D. https://doi.org/10.1039/d0cp00897d

Author

Newland, Mike ; Nelson, Bethany ; Muñoz, Amalia ; Ródenas, Milagros ; Vera, Teresa ; Tárrega, Joan ; Rickard, Andrew Robert. / Trends in stabilisation of Criegee intermediates from alkene ozonolysis. In: Physical Chemistry Chemical Physics. 2020 ; Vol. 22. pp. 13698-13706.

Bibtex - Download

@article{1b54c525bf0a4d548b7e03b58cd4eb86,
title = "Trends in stabilisation of Criegee intermediates from alkene ozonolysis",
abstract = "Criegee Intermediates (CI), formed in the ozonolysis of alkenes, play a central role in tropospheric chemistry as an important source of radicals, with stabilised CI (SCI) able to participate in bimolecular reactions, affecting climate through the formation of inorganic and organic aerosol. However, total SCI yields have only been determined for a few alkene systems, while speciated SCI yields from asymmetrical alkenes are almost entirely unknown. Here we report for the first time a systematic experimental exploration of the stabilisation of CH2OO and (CH3)2COO CI, formed from ten alkene–ozone systems with a range of different sizes and structures, under atmospherically relevant conditions in the EUPHORE chamber. Experiments in the presence of excess SO2 (an SCI scavenger) determined total SCI yields from each alkene–ozone system. Comparison of primary carbonyl yields in the presence/absence of SO2 determined the stabilisation fraction of a given CI. The results show that the stabilisation of a given CI increases as the size of the carbonyl co-product increases. This is interpreted in terms of the nascent population of CI formed following decomposition of the primary ozonide (POZ) having a lower mean energy distribution when formed with a larger carbonyl co-product, as more of the energy from the POZ is taken by the carbonyl. These findings have significant implications for atmospheric modelling of alkene ozonolysis. Higher stabilisation of small CI formed from large alkenes is expected to lead to lower radical yields from CI decomposition, and higher SCI concentrations, increasing the importance of SCI bimolecular reactions.",
keywords = "Atmospheric Chemistry, Chemical Kinetics, CHEMICAL MECHANISM DEVELOPMENT, Criegee intermediate, Ozonolysis",
author = "Mike Newland and Bethany Nelson and Amalia Mu{\~n}oz and Milagros R{\'o}denas and Teresa Vera and Joan T{\'a}rrega and Rickard, {Andrew Robert}",
note = "{\textcopyright} the Owner Societies 2020",
year = "2020",
month = jun,
day = "4",
doi = "10.1039/d0cp00897d",
language = "English",
volume = "22",
pages = "13698--13706",
journal = "Physical Chemistry Chemical Physics",
issn = "1463-9076",
publisher = "The Royal Society of Chemistry",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Trends in stabilisation of Criegee intermediates from alkene ozonolysis

AU - Newland, Mike

AU - Nelson, Bethany

AU - Muñoz, Amalia

AU - Ródenas, Milagros

AU - Vera, Teresa

AU - Tárrega, Joan

AU - Rickard, Andrew Robert

N1 - © the Owner Societies 2020

PY - 2020/6/4

Y1 - 2020/6/4

N2 - Criegee Intermediates (CI), formed in the ozonolysis of alkenes, play a central role in tropospheric chemistry as an important source of radicals, with stabilised CI (SCI) able to participate in bimolecular reactions, affecting climate through the formation of inorganic and organic aerosol. However, total SCI yields have only been determined for a few alkene systems, while speciated SCI yields from asymmetrical alkenes are almost entirely unknown. Here we report for the first time a systematic experimental exploration of the stabilisation of CH2OO and (CH3)2COO CI, formed from ten alkene–ozone systems with a range of different sizes and structures, under atmospherically relevant conditions in the EUPHORE chamber. Experiments in the presence of excess SO2 (an SCI scavenger) determined total SCI yields from each alkene–ozone system. Comparison of primary carbonyl yields in the presence/absence of SO2 determined the stabilisation fraction of a given CI. The results show that the stabilisation of a given CI increases as the size of the carbonyl co-product increases. This is interpreted in terms of the nascent population of CI formed following decomposition of the primary ozonide (POZ) having a lower mean energy distribution when formed with a larger carbonyl co-product, as more of the energy from the POZ is taken by the carbonyl. These findings have significant implications for atmospheric modelling of alkene ozonolysis. Higher stabilisation of small CI formed from large alkenes is expected to lead to lower radical yields from CI decomposition, and higher SCI concentrations, increasing the importance of SCI bimolecular reactions.

AB - Criegee Intermediates (CI), formed in the ozonolysis of alkenes, play a central role in tropospheric chemistry as an important source of radicals, with stabilised CI (SCI) able to participate in bimolecular reactions, affecting climate through the formation of inorganic and organic aerosol. However, total SCI yields have only been determined for a few alkene systems, while speciated SCI yields from asymmetrical alkenes are almost entirely unknown. Here we report for the first time a systematic experimental exploration of the stabilisation of CH2OO and (CH3)2COO CI, formed from ten alkene–ozone systems with a range of different sizes and structures, under atmospherically relevant conditions in the EUPHORE chamber. Experiments in the presence of excess SO2 (an SCI scavenger) determined total SCI yields from each alkene–ozone system. Comparison of primary carbonyl yields in the presence/absence of SO2 determined the stabilisation fraction of a given CI. The results show that the stabilisation of a given CI increases as the size of the carbonyl co-product increases. This is interpreted in terms of the nascent population of CI formed following decomposition of the primary ozonide (POZ) having a lower mean energy distribution when formed with a larger carbonyl co-product, as more of the energy from the POZ is taken by the carbonyl. These findings have significant implications for atmospheric modelling of alkene ozonolysis. Higher stabilisation of small CI formed from large alkenes is expected to lead to lower radical yields from CI decomposition, and higher SCI concentrations, increasing the importance of SCI bimolecular reactions.

KW - Atmospheric Chemistry

KW - Chemical Kinetics

KW - CHEMICAL MECHANISM DEVELOPMENT

KW - Criegee intermediate

KW - Ozonolysis

U2 - 10.1039/d0cp00897d

DO - 10.1039/d0cp00897d

M3 - Article

VL - 22

SP - 13698

EP - 13706

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

M1 - D0CP00897D

ER -