American Chemical Society
jz2c02734_si_003.mpg (4.58 MB)

Promoted Activity of Surface Hydroxyls on γ‑Al2O3 Mineral Dust with the Coexistence of SO2 and NH3

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Version 2 2022-11-02, 17:09
Version 1 2022-10-31, 12:10
posted on 2022-11-02, 17:09 authored by Hao Li, Haobo Xue, Biwu Chu, Qingxin Ma, Hong He
Sulfate and ammonium formed on mineral dust can be mutually accelerated through the heterogeneous reactions of coexisting SO2 and NH3. However, little is known about the underlying mechanism, especially the pivotal reactive sites. Using combined Born–Oppenheimer molecular dynamics simulations and density functional theory calculations, the results show that, compared to that of SO2 or NH3 alone on the γ-Al2O3 surface, the increased level of formation of sulfate and ammonium can be attributed to the promoted activity of the surface-bridged hydroxyl with the coexistence of SO2 and NH3. In the specific mechanism, the O and H of the surface-bridged hydroxyl group are attacked by the adjacent SO2 and NH3, respectively, which directly enhances the formation of absorbed sulfite and ammonium, and indirectly facilitates the production of sulfate by oxidation of atmospheric O2. The proposed mechanisms can be broadly applied to other aluminum-based suspended dust particles, such as kaolinite, montmorillonite, and clay dust.