Interactions between natural mineral dust and methylglyoxal: a Knudsen flow reactor study
Résumé
Atmospheric aerosols have a significant impact on climate. They influence the direct radiative forcing by
scattering or absorbing solar radiations. They also act as cloud condensation nuclei. Atmospheric aerosols can
interact with gas-phase species by providing surfaces for their uptake. This process can modify the surface of
aerosols, so-called chemical aging. Mineral dust, is the main component of the global atmospheric aerosol mass
budget. They account approximately for half of the annual particle emissions. Dust particles can travel several
thousands of kilometers and impact areas far from their origin. Despite the importance of mineral dust in the
atmosphere, large uncertainties remain regarding their impact on climate and air quality. This is mainly due to
the poor understanding of the fate of dust in the atmosphere, and of the underlying chemical process they allow.
The objective of this study is to investigate the uptake of methylglyoxal on natural mineral dust surfaces. This
dicarbonyl compound is produced by isoprene oxidation in the atmosphere. It is considered an important
precursor of secondary organic aerosols (SOA), and thus its atmospheric fate has significant implications for
Earth’s climate. Uptake experiments are performed in a Knudsen flow reactor, operated in the molecular flow
regime, and coupled with a modulated molecular beam quadrupole mass spectrometer for real-time monitoring
of the gas-phase reactants and products. To characterize the heterogeneous interactions of methylglyoxal with a
selection of representative mineral surrogates, initial uptake coefficients (γ0) and surface coverages (Ns) are
determined.
Experiments evidence high initial uptakes of methylglyoxal on the selected natural desert dusts, ranging from
0.1 to 0.2. The total number of molecules adsorbed at the surface of dust samples ranges from 9.5×1013 to
28.5×1013 molecule cm-2. A correlation between the number of molecules adsorbed on the surface and the
elemental composition of dusts is presented and discussed. Desorption is investigated at ambient temperature.
No desorption is evidenced, pointing to the irreversible nature of methylglyoxal uptake on selected dusts at
tropospheric temperature.
The use of various natural dust samples from contrasted origins provides a trend of methylglyoxal uptake on
desert dust samples. The comparison with the elemental composition allows pointing at the contribution of
specific elements on the uptake. These results provide new insights into the fate of methylglyoxal in the
atmosphere and allow a wider view of the atmospheric sinks of Methylglyoxal in the atmosphere.