Issue 11, 2022

The dependence of soot particle ice nucleation ability on its volatile content

Abstract

Aviation soot can affect contrail and cirrus cloud formation and impact climate. A product of incomplete combustion, soot particles, are fractal and hydrophobic aggregates comprising carbonaceous spheres with complex physicochemical properties. In the cirrus cloud regime, the surface wettability and pore abundance of soot particles are important determinants for their ice nucleation ability via pore condensation and freezing. In the atmosphere, soot particles can undergo various ageing processes which modify their surface chemistry and porosity, thus acting as ice nucleating particles with varying abilities as a function of ageing. In this study, size-selected soot particles were treated by thermal denuding at 573 K in a pure nitrogen (N2) or synthetic air (N2 + O2) flow and then exposed to varying relative humidity conditions at a fixed temperature in the range from 218 to 243 K, to investigate the role of volatile content in the ice nucleation ability. Both organic-lean and organic-rich propane (C3H8) flame soot particles, as well as two types of commercially available carbon black soot particles with high and low surface wettability, were tested. The size and mass distribution of soot aerosol were monitored during the ice nucleation experiments. Bulk soot samples also prepared in pure N2 or synthetic air environments at 573 K were characterised by thermogravimetric analysis, Fourier transform infrared spectroscopy and dynamic vapour sorption measurements, to reveal the relation between denuding volatile content, associated soot particle property modifications and the ice nucleation ability. Our study shows that thermal denuding induces a change in soot particle porosity playing a dominant role in regulating its ice nucleation via the pore condensation and freezing mechanism. The enrichment in mesopore (2–50 nm) availability may enhance soot ice nucleation. The presence of O2 in the thermal denuding process may introduce new active sites on soot particles for water interaction and increase soot surface wettability. However, these active sites only facilitate soot ice nucleation when mesopore structures are available. We conclude that a change in volatile content modifies both morphological properties and surface chemistry for soot particles, but porosity change plays the dominant role in regulating soot particle ice nucleation ability.

Graphical abstract: The dependence of soot particle ice nucleation ability on its volatile content

Supplementary files

Article information

Article type
Paper
Submitted
15 Apr. 2022
Accepted
10 Aug. 2022
First published
17 Aug. 2022
This article is Open Access
Creative Commons BY-NC license

Environ. Sci.: Processes Impacts, 2022,24, 2043-2069

The dependence of soot particle ice nucleation ability on its volatile content

K. Gao, H. Koch, C. Zhou and Z. A. Kanji, Environ. Sci.: Processes Impacts, 2022, 24, 2043 DOI: 10.1039/D2EM00158F

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