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. Iron-containing mineral aerosols play a key role in the oxidationof sulfur species in the atmosphere. Simulated cloud processing (CP) oftypical mineral particles, such as illite (IMt-2), nontronite (NAu-2),smectite (SWy-2) and Arizona Test Dust (ATD) is shown here to modify sulfurdioxide ( SO2 ) uptake onto mineral surfaces. Heterogeneous oxidation of SO2 on particle surfaces was firstly investigated using an in situ DRIFTSapparatus (diffuse reflectance infrared Fourier transform spectroscopy). Our results showed that the Brunauer–Emmett–Teller (BET) surface area normalized uptakecoefficients ( γBET ) of SO2 on the IMt-2, NAu-2, SWy-2 andATD samples after CP were 2.2, 4.1, 1.5 and 1.4 times higher than thecorresponding ones before CP, respectively. The DRIFTS results suggestedthat CP increased the amounts of reactive sites (e.g., surface OH groups) onthe particle surfaces and thus enhanced the uptake of SO2 . Transmissionelectron microscopy (TEM) showedthat the particles broke up into smaller pieces after CP, and thus producedmore active sites. The “free-Fe” measurements confirmed that more reactiveFe species were present after CP, which could enhance the SO2 uptakemore effectively. Mossbauer spectroscopy further revealedthat the formed Fe phases were amorphous Fe(III) and nanosized ferrihydritehybridized with Al  ∕  Si, which were possibly transformed from the Fe in thealuminosilicate lattice. The modification of Fe speciation was driven by thepH-dependent fluctuation coupling with Fe dissolution–precipitationcycles repeatedly during the experiment. Considering both the enhanced SO2 uptake and subsequent promotion of iron dissolution along with more activeFe formation, which in turn led to more SO2 uptake, it was proposedthat there may be a positive feedback between SO2 uptake and ironmobilized on particle surfaces during CP, thereby affecting climate andbiogeochemical cycles. This self-amplifying mechanism generated on theparticle surfaces may also serve as the basis of high sulfate loading insevere fog–haze events observed recently in China.

Enhanced heterogeneous uptake of sulfur dioxide on mineral particles through modification of iron speciation during simulated cloud processing