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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 05 Jun 2019

Submitted as: research article | 05 Jun 2019

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This discussion paper is a preprint. A revision of the manuscript is under review for the journal Atmospheric Chemistry and Physics (ACP).

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

Zhenzhen Wang1, Tao Wang1, Hongbo Fu1,2,3, Liwu Zhang1, Mingjin Tang4, Christian George5, Vicki H. Grassian6, and Jianmin Chen1 Zhenzhen Wang et al.
  • 1Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science & Engineering, Institute of Atmospheric Sciences, Fudan University, Shanghai, 200433, China
  • 2Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
  • 3Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET), Nanjing University of Information Science and Technology, Nanjing 210044, China
  • 4State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
  • 5University of Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, F-69626, Villeurbanne, France
  • 6Departments of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92093, United States

Abstract. 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. Our results showed that the 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. 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 phase 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 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 lead 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.

Zhenzhen Wang et al.
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Status: final response (author comments only)
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Zhenzhen Wang et al.
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Short summary
This study confirmed that SO2 uptake on the mineral particles could be greatly enhanced during cloud processing. The large pH fluctuations between the cloud-aerosol modes could significantly modify the microphysical properties of particles, and triggered formation of reactive Fe particles to accelerate sulfate formation via a self-amplifying process. Results of this study could partly explain the missing source of sulfate and improve agreement between models and field observations.
This study confirmed that SO2 uptake on the mineral particles could be greatly enhanced during...