气候变化领域集成服务门户(CCPortal): Enhanced heterogeneous uptake of sulfur dioxide on mineral particles through modification of iron speciation during simulated cloud processing

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DOI	10.5194/acp-19-12569-2019
	Enhanced heterogeneous uptake of sulfur dioxide on mineral particles through modification of iron speciation during simulated cloud processing
	Wang Z.; Wang T.; Fu H.; Zhang L.; Tang M.; George C.; Grassian V.H.; Chen J.
发表日期	2019
ISSN	16807316
起始页码	12569
结束页码	12585
卷号	19 期号:19
英文摘要	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. © Author(s) 2019.
语种	英语
scopus关键词	aerosol; aerosol composition; fog; haze; heterogeneity; iron; oxidation; particulate matter; speciation (chemistry); sulfur dioxide; China
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/144101
作者单位	Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Institute of Atmospheric Sciences, Fudan University, Shanghai, 200433, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, China; Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET), Nanjing University of Information Science and Technology, Nanjing, 210044, China; State Key Lab. of Organ. Geochem. and Guangdong Key Lab. of Environ. Protect. and Rsrc. Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, 510640, China; University of Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, Villeurbanne, 69626, France; Department of Chemistry and Biochemistry, University of California, San Diego, San Diego, CA 92093, United States
推荐引用方式 GB/T 7714	Wang Z.,Wang T.,Fu H.,et al. Enhanced heterogeneous uptake of sulfur dioxide on mineral particles through modification of iron speciation during simulated cloud processing[J],2019,19(19).
APA	Wang Z..,Wang T..,Fu H..,Zhang L..,Tang M..,...&Chen J..(2019).Enhanced heterogeneous uptake of sulfur dioxide on mineral particles through modification of iron speciation during simulated cloud processing.Atmospheric Chemistry and Physics,19(19).
MLA	Wang Z.,et al."Enhanced heterogeneous uptake of sulfur dioxide on mineral particles through modification of iron speciation during simulated cloud processing".Atmospheric Chemistry and Physics 19.19(2019).