Abstract
The uptake of O3 (1 × 1012–5× 1013 cm−3) on a methane soot coating preliminarily exposed to N2O5, is studied using a flow reactor with a movable insert. Based on the dependence of the ozone uptake coefficient on the exposure time and O3 concentration, the uptake mechanism is established and a number of elementary parameters are obtained that describe the uptake process at arbitrary O3 concentrations. Based on the Langmuir representation of adsorption, a model description of the uptake on soot under conditions of the competitive adsorption of O3/NOx, where NOx = NO2 and N2O5, taking into account the multistage uptake process, is proposed. Based on the developed model and elementary parameters describing the uptake of O3, NO2, and N2O5 on a fresh soot surface, as well as the uptake of ozone on a surface pretreated with NO2 and N2O5, numerical estimates were made of the additional contributions to the ozone uptake for two real scenarios of the O3/NOx ratio. For an industrial region in winter, when the ozone concentration is minimal (10 ppb O3, 17 ppb NO2, and 4 ppb N2O5), the additional integral contribution to the uptake of O3 on the reaction products of NO2 with soot is 68%, and in the case of N2O5, it is 3.6%. For the same region in summer, at the maximum ozone concentration (36 ppb O3, 17 ppb NO2, and 4 ppb N2O5), the analogous contributions will be 20 and 1%, respectively. The reasons for this difference are discussed.
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1134%2FS1990793123010141/MediaObjects/11826_2023_8738_Fig1_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1134%2FS1990793123010141/MediaObjects/11826_2023_8738_Fig2_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1134%2FS1990793123010141/MediaObjects/11826_2023_8738_Fig3_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1134%2FS1990793123010141/MediaObjects/11826_2023_8738_Fig4_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1134%2FS1990793123010141/MediaObjects/11826_2023_8738_Fig5_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1134%2FS1990793123010141/MediaObjects/11826_2023_8738_Fig6_HTML.png)
REFERENCES
E. E. McDuffie, D. L. Fibiger, W. P. Dubé, et al., J. Geophys. Res. Atmos. 123, 4345 (2018). https://doi.org/10.1002/2018JD028336
I. K. Larin, Russian J. Phys. Chem. B 13 (3), 548 (2019). https://doi.org/10.1134/S1990793119030084
I. K. Larin, A. E. Aloyan, and A. N. Ermakov, Russian J. Phys. Chem. B 15 (3), 577 (2021). https://doi.org/10.1134/S199079312103009X
W. L. Chang, P. V. Bhave, S. S. Brown, et al., Aerosol Sci. Technol. 45, 665 (2011). https://doi.org/10.1080/02786826.2010.551672
L. Jaeglé, V. Shah, J. A. Thornton, et al., J. Geophys. Res. Atmos. 123, 12368 (2018). https://doi.org/10.1029/2018JD029133
R. A. Washenfelder, N. L. Wagner, W. P. Dubé, and S. S. Brown, Environ. Sci. Technol. 45, 2938 (2011). https://doi.org/10.1021/es10334u
Z. Liu, R. M. Doherty, O. Wild, et al., Atmos. Chem. Phys. 22, 1209 (2022). https://doi.org/10.5194/acp-22-1209-2022
D. Roberts-Semple, F. Song, and Yu. Gao, Atmos. Pollut. Res. 3, 247 (2012). https://www.atmospolres.com.
N. L. Wagner, T. P. Riedel, C. J. Young, et al., J. Geophys. Res. 118D, 9331 (2013). https://doi.org/10.1002/jgrd.50653
A. Berner, S. Sidla, Z. Galambos, et al., J. Geophys. Res. Atmos. 101, 19559 (1996). https://doi.org/10.1029/95JD03425
K. Pohl, M. Cantwell, P. Herckes, and R. Lohmann, Atmos. Chem. Phys. 14, 7431 (2014). https://doi.org/10.5194/acp-14-7431-2014,2014
T. C. Bond, D. G. Streets, K. F. Yarber, et al., J. Geophys. Res. 109, D14203 (2004). https://doi.org/10.1029/2003JD003697
R. Wang, S. Tao, H. Shen, et al., Environ. Sci. Technol. 48, 6780 (2014). https://doi.org/10.1021/es5021422
Z. Klimont, K. Kupiainen, C. Heyes, et al., Atmos. Chem. Phys. 17, 8681 (2017). https://doi.org/10.5194/acp-8681-2017
J. B. Burkholder, S. P. Sander, J. P. D. Abbatt, et al., “Chemical kinetics and photochemical data for use in atmospheric studies, evaluation no. 19,” NASA JPL Publication 19-5, Pasadena (2019). http://jpldataeval.jpl.nasa.gov.
S. Kamm, O. Möhler, K.-H. Naumann, et al., Atmos. Environ. 33, 4651 (1999).
A. R. Chughtai, J. M. Kim, and D. M. Smith, J. Atmos. Chem. 45, 231 (2003). https://doi.org/10.1023/A:1024250505886
V. V. Zelenov and E. V. Aparina, Russian J. Phys. Chem. B 15 (3), 547 (2021). https://doi.org/10.1134/S1990793121030143
V. V. Zelenov and E. V. Aparina, Russian J. Phys. Chem. B 15 (5), 919 (2021). https://doi.org/10.1134/S199079312050225
V. V. Zelenov and E. V. Aparina, Russian J. Phys. Chem. B 16 (6), 1182 (2022). https://doi.org/10.1134/S1990793122060239
F. Karagulian and M. J. Rossi, J. Phys. Chem. A 111, 1914 (2007). https://doi.org/10.1021/jp0670891
T. Moise and Y. Rudich, J. Geophys. Res. 105D, 14667 (2000). doi 0148-0227/00/2000JD900071
M. Ammann, U. Pöschl, and Y. Rudich, Phys. Chem. Chem. Phys. 5, 351 (2003). https://doi.org/10.1039/b208708a
U. Pöschl, Y. Rudich, and M. Ammann, Atmos. Chem. Phys. 7, 5989 (2007). https://www.atmos-chemphys.net/7/5989/2007/.
Funding
This study was performed as part of the state task FFZE-2022-0008 (registration no. 1021051302551-2-1.3.1; 1.4.7; 1.6.19).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Zelenov, V.V., Aparina, E.V. Modeling the Time-Dependent O3 Uptake on a Methane Flame Soot Coating Under Conditions of Competitive O3/NO2 and O3/N2O5 Adsorption. Russ. J. Phys. Chem. B 17, 234–243 (2023). https://doi.org/10.1134/S1990793123010141
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1134/S1990793123010141