Rate Acceleration of the Heterogeneous Reaction of Ozone with a
Model Alkene at the Air-Ice Interface at Low Temperatures

J 2013

Rate Acceleration of the Heterogeneous Reaction of Ozone with a Model Alkene at the Air-Ice Interface at Low Temperatures

RAY, Debajyoti, Joseph K'ekuboni MALONGWE and Petr KLÁN

Basic information

Original name

Rate Acceleration of the Heterogeneous Reaction of Ozone with a Model Alkene at the Air-Ice Interface at Low Temperatures

Authors

RAY, Debajyoti (356 India, belonging to the institution), Joseph K'ekuboni MALONGWE (180 Democratic Republic of the Congo, belonging to the institution) and Petr KLÁN (203 Czech Republic, guarantor, belonging to the institution)

Edition

Environmental Science and Technology, Columbus, Ohio, USA, American Chemical Society, 2013, 0013-936X

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

10401 Organic chemistry

Country of publisher

United States of America

Confidentiality degree

není předmětem státního či obchodního tajemství

References:

URL

Impact factor

Impact factor: 5.481

RIV identification code

RIV/00216224:14310/13:00066641

Organization unit

Faculty of Science

DOI

http://dx.doi.org/10.1021/es304812t

UT WoS

000321521400009

Keywords in English

Photochemistry; Ice; Snow; Ozone

Abstract

V originále

The kinetics of the ozonation reaction of 1,1-diphenylethylene (DPE) on the surface of ice grains (also called "artificial snow"), produced by shock-freezing of DPE aqueous solutions or DPE vapor-deposition on pure ice grains, was studied in the temperature range of 268 to 188 K. A remarkable and unexpected increase in the apparent ozonation rates with decreasing temperature was evaluated using the Langmuir-Hinshelwood and Eley-Rideal kinetic models, and by estimating the apparent specific surface area of the ice grains. We suggest that an increase of the number of surface reactive sites, and possibly higher ozone uptake coefficients are responsible for the apparent rate acceleration of DPE zonation at the air ice interface at lower temperatures. The increasing number of reactive sites is probably related to the fact that organic molecules are displaced more to the top of a disordered interface (or quasi liquid) layer on the ice surface, which makes them more accessible to the gas phase reactants. The effect of NaCl as a cocontaminant on ozonation rates was also investigated. The environmental implications of this phenomenon for natural ice/snow are discussed. DPE was selected as an example of environmentally relevant species which can react with ozone. For typical atmospheric ozone concentrations in polar areas (20 ppbv), we estimated that its half-life on the ice surface would decrease from similar to 5 days at 258 K to similar to 13 h at 188 K at submonolayer DPE loadings.

Links

ED0001/01/01, research and development project

Name: CETOCOEN

GAP503/10/0947, research and development project

Name: Důsledky fotochemické aktivity organických polutantů v polárních oblastech

Investor: Czech Science Foundation

LM2011028, research and development project

Name: RECETOX ? Národní infrastruktura pro výzkum toxických látek v prostředí

Investor: Ministry of Education, Youth and Sports of the CR

Citovat

RAY, Debajyoti, Joseph K'ekuboni MALONGWE and Petr KLÁN. Rate Acceleration of the Heterogeneous Reaction of Ozone with a Model Alkene at the Air-Ice Interface at Low Temperatures. Environmental Science and Technology. Columbus, Ohio, USA: American Chemical Society, 2013, vol. 47, No 13, p. 6773-6780. ISSN 0013-936X. Available from: https://dx.doi.org/10.1021/es304812t.

@article{1138371,
   author = {Ray, Debajyoti and Malongwe, Joseph K'ekuboni and Klán, Petr},
   article_location = {Columbus, Ohio, USA},
   article_number = {13},
   doi = {http://dx.doi.org/10.1021/es304812t},
   keywords = {Photochemistry; Ice; Snow; Ozone},
   language = {eng},
   issn = {0013-936X},
   journal = {Environmental Science and Technology},
   title = {Rate Acceleration of the Heterogeneous Reaction of Ozone with a Model Alkene at the Air-Ice Interface at Low Temperatures},
   url = {http://pubs.acs.org/doi/abs/10.1021/es304812t},
   volume = {47},
   year = {2013}
}

TY  - JOUR
ID  - 1138371
AU  - Ray, Debajyoti - Malongwe, Joseph K'ekuboni - Klán, Petr
PY  - 2013
TI  - Rate Acceleration of the Heterogeneous Reaction of Ozone with a Model Alkene at the Air-Ice Interface at Low Temperatures
JF  - Environmental Science and Technology
VL  - 47
IS  - 13
SP  - 6773-6780
EP  - 6773-6780
PB  - American Chemical Society
SN  - 0013936X
KW  - Photochemistry
KW  - Ice
KW  - Snow
KW  - Ozone
UR  - http://pubs.acs.org/doi/abs/10.1021/es304812t
L2  - http://pubs.acs.org/doi/abs/10.1021/es304812t
N2  - The kinetics of the ozonation reaction of 1,1-diphenylethylene (DPE) on the surface of ice grains (also called "artificial snow"), produced by shock-freezing of DPE aqueous solutions or DPE vapor-deposition on pure ice grains, was studied in the temperature range of 268 to 188 K. A remarkable and unexpected increase in the apparent ozonation rates with decreasing temperature was evaluated using the Langmuir-Hinshelwood and Eley-Rideal kinetic models, and by estimating the apparent specific surface area of the ice grains. We suggest that an increase of the number of surface reactive sites, and possibly higher ozone uptake coefficients are responsible for the apparent rate acceleration of DPE zonation at the air ice interface at lower temperatures. The increasing number of reactive sites is probably related to the fact that organic molecules are displaced more to the top of a disordered interface (or quasi liquid) layer on the ice surface, which makes them more accessible to the gas phase reactants. The effect of NaCl as a cocontaminant on ozonation rates was also investigated. The environmental implications of this phenomenon for natural ice/snow are discussed. DPE was selected as an example of environmentally relevant species which can react with ozone. For typical atmospheric ozone concentrations in polar areas (20 ppbv), we estimated that its half-life on the ice surface would decrease from similar to 5 days at 258 K to similar to 13 h at 188 K at submonolayer DPE loadings.
ER  -

RAY, Debajyoti, Joseph K'ekuboni MALONGWE and Petr KLÁN. Rate Acceleration of the Heterogeneous Reaction of Ozone with a Model Alkene at the Air-Ice Interface at Low Temperatures. \textit{Environmental Science and Technology}. Columbus, Ohio, USA: American Chemical Society, 2013, vol.~47, No~13, p.~6773-6780. ISSN~0013-936X. Available from: https://dx.doi.org/10.1021/es304812t.

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