Impact of greenhouse gas CO2 on the heterogeneous reaction of SO2 on alpha-Al2O3 |
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| Affiliation: | 1. State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China;2. POTEN Environment Group Co., Ltd., Beijing 100082, China;1. State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, PR China;2. University of Chinese Academy of Sciences, Beijing 100049, PR China;3. Center for Excellence in Urban Atmospheric Environment (CEUAE), Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, PR China;1. College of Resource and Environment Sciences, Xinjiang University, Urumqi 830046, PR China;2. Institute of Chemical Physics, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, PR China |
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| Abstract: | The heterogeneous reaction of SO2 on mineral dust surfaces is generally considered as an important chemical pathway for secondary sulfate formation in the troposphere. To this day, there are no reported studies that assess the impact of atmospheric CO2 in sulfate production on mineral dust surfaces. In this work, we investigate the impact of CO2 on SO2 uptake on dust proxy aluminum oxide particles using a diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). CO2 is demonstrated to suppress the heterogeneous oxidation of SO2 on alpha-Al2O3. Compared to that measured in the CO2-free case, the uptake coefficient is decreased by nearly 57% when Al2O3 particles are exposed to the gas flow with atmospheric CO2 at a relative humidity (RH) of 25%. It is also found that there is a balance between the yield of active moiety −OH provided by Al(OH)3(CO)(OH)2 clusters and the loss of basic hydroxyl group on aluminum oxide surfaces blocked by CO2-derived (bi)carbonate species. This work, for the first time, reveals a negative effect of atmospheric CO2 on the sulfate formation, which potentially decreases solar-radiation scattering and further exacerbates global warming. |
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| Keywords: | Sulfate Mineral dust Heterogeneous reaction |
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