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Iron-containing mineral aerosols play a key role in the oxidation of sulfur species in the atmosphere. Simulated cloud processing (CP) of typical mineral particles, such as illite (IMt-2), nontronite (NAu-2), smectite (SWy-2) and Arizona Test Dust (ATD) is shown here to modify sulfur dioxide (SO2) uptake onto mineral surfaces. Heterogeneous oxidation of SO2 on particle surfaces was firstly investigated using an in situ DRIFTS apparatus (diffuse reflectance infrared Fourier transform spectroscopy). Our results showed that the Brunauer–Emmett–Teller (BET) surface area normalized uptake coefficients (γBET) of SO2 on the IMt-2, NAu-2, SWy-2 and ATD samples after CP were 2.2, 4.1, 1.5 and 1.4 times higher than the corresponding ones before CP, respectively. The DRIFTS results suggested that CP increased the amounts of reactive sites (e.g., surface OH groups) on the particle surfaces and thus enhanced the uptake of SO2. Transmission electron microscopy (TEM) showed that the particles broke up into smaller pieces after CP, and thus produced more active sites. The "free-Fe" measurements confirmed that more reactive Fe species were present after CP, which could enhance the SO2 uptake more effectively. Mössbauer spectroscopy further revealed that the formed Fe phases were amorphous Fe(III) and nanosized ferrihydrite hybridized with Al / Si, which were possibly transformed from the Fe in the aluminosilicate lattice. The modification of Fe speciation was driven by the pH-dependent fluctuation coupling with Fe dissolution–precipitation cycles repeatedly during the experiment. Considering both the enhanced SO2 uptake and subsequent promotion of iron dissolution along with more active Fe formation, which in turn led to more SO2 uptake, it was proposed that there may be a positive feedback between SO2 uptake and iron mobilized on particle surfaces during CP, thereby affecting climate and biogeochemical cycles. This self-amplifying mechanism generated on the particle surfaces may also serve as the basis of high sulfate loading in severe fog–haze events observed recently in China. [ABSTRACT FROM AUTHOR]