Using Nanoparticle X-ray Spectroscopy to Probe the Formation of Reactive Chemical Gradients in Diffusion-Limited Aerosols
Abstract
For aerosol particles that exist in highly viscous, diffusion-limited states, steep chemical gradients are expected to form during photochemical aging in the atmosphere. Under these conditions, species at the aerosol surface are more rapidly transformed than molecules residing in the particle interior. To examine the formation and evolution of chemical gradients at aerosol interfaces, the heterogeneous reaction of hydroxyl radicals (OH) on ~200 nm particles of pure squalane (a branched, liquid hydrocarbon) and octacosane (a linear, solid hydrocarbon) and binary mixtures of the two are used to understand how diffusion limitations and phase separation impact the particle reactivity. Aerosol mass spectrometry is used to measure the effective heterogeneous OH uptake coefficient (γeff) and oxidation kinetics in the bulk, which are compared with the elemental composition of the surface obtained using X-ray photoemission. When diffusion rates are fast relative to the reaction frequency, as is the case for squalane and low-viscosity squalane–octacosane mixtures, the reaction is efficient (γeff ~ 0.3) and only limited by the arrival of OH to the interface. However, for cases, where the diffusion rates are slower than reaction rates, as in pure octacosane and higher-viscosity squalane–octacosane mixtures, the heterogeneous reaction occurs in a mixing-limited regime and ismore »
- Authors:
-
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1608272
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
- Additional Journal Information:
- Journal Volume: 123; Journal Issue: 28; Journal ID: ISSN 1089-5639
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Jacobs, Michael I., Xu, Bo, Kostko, Oleg, Wiegel, Aaron A., Houle, Frances A., Ahmed, Musahid, and Wilson, Kevin R. Using Nanoparticle X-ray Spectroscopy to Probe the Formation of Reactive Chemical Gradients in Diffusion-Limited Aerosols. United States: N. p., 2019.
Web. doi:10.1021/acs.jpca.9b04507.
Jacobs, Michael I., Xu, Bo, Kostko, Oleg, Wiegel, Aaron A., Houle, Frances A., Ahmed, Musahid, & Wilson, Kevin R. Using Nanoparticle X-ray Spectroscopy to Probe the Formation of Reactive Chemical Gradients in Diffusion-Limited Aerosols. United States. https://doi.org/10.1021/acs.jpca.9b04507
Jacobs, Michael I., Xu, Bo, Kostko, Oleg, Wiegel, Aaron A., Houle, Frances A., Ahmed, Musahid, and Wilson, Kevin R. Fri .
"Using Nanoparticle X-ray Spectroscopy to Probe the Formation of Reactive Chemical Gradients in Diffusion-Limited Aerosols". United States. https://doi.org/10.1021/acs.jpca.9b04507. https://www.osti.gov/servlets/purl/1608272.
@article{osti_1608272,
title = {Using Nanoparticle X-ray Spectroscopy to Probe the Formation of Reactive Chemical Gradients in Diffusion-Limited Aerosols},
author = {Jacobs, Michael I. and Xu, Bo and Kostko, Oleg and Wiegel, Aaron A. and Houle, Frances A. and Ahmed, Musahid and Wilson, Kevin R.},
abstractNote = {For aerosol particles that exist in highly viscous, diffusion-limited states, steep chemical gradients are expected to form during photochemical aging in the atmosphere. Under these conditions, species at the aerosol surface are more rapidly transformed than molecules residing in the particle interior. To examine the formation and evolution of chemical gradients at aerosol interfaces, the heterogeneous reaction of hydroxyl radicals (OH) on ~200 nm particles of pure squalane (a branched, liquid hydrocarbon) and octacosane (a linear, solid hydrocarbon) and binary mixtures of the two are used to understand how diffusion limitations and phase separation impact the particle reactivity. Aerosol mass spectrometry is used to measure the effective heterogeneous OH uptake coefficient (γeff) and oxidation kinetics in the bulk, which are compared with the elemental composition of the surface obtained using X-ray photoemission. When diffusion rates are fast relative to the reaction frequency, as is the case for squalane and low-viscosity squalane–octacosane mixtures, the reaction is efficient (γeff ~ 0.3) and only limited by the arrival of OH to the interface. However, for cases, where the diffusion rates are slower than reaction rates, as in pure octacosane and higher-viscosity squalane–octacosane mixtures, the heterogeneous reaction occurs in a mixing-limited regime and is ~10× slower (γeff ~ 0.03). This is in contrast to carbon and oxygen K edge X-ray absorption measurements that show that the octacosane interface is oxidized much more rapidly than that of pure squalane particles. The O/C ratio of the surface (estimated to be the top 6–8 nm of the interface) is measured to change with rate constants of (3.0 ± 0.9) × 10–13 and (8.6 ± 1.2) × 10–13 cm3 molecule–1 s–1 for squalane and octacosane particles, respectively. The differences in surface oxidation rates are analyzed using a previously published reaction-diffusion model, which suggests that a 1–2 nm highly oxidized crust forms on octacosane particles, whereas in pure squalane, the reaction products are homogeneously mixed within the aerosol. This work illustrates how diffusion limitations can form particles with highly oxidized surfaces even at relatively low oxidant exposures, which is in turn expected to influence their microphysics in the atmosphere.},
doi = {10.1021/acs.jpca.9b04507},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 28,
volume = 123,
place = {United States},
year = {Fri Jun 21 00:00:00 EDT 2019},
month = {Fri Jun 21 00:00:00 EDT 2019}
}
Web of Science
Figures / Tables:
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