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DOI10.5194/acp-22-6045-2022
Iron from coal combustion particles dissolves much faster than mineral dust under simulated atmospheric acidic conditions
Baldo, Clarissa; Ito, Akinori; Krom, Michael D.; Li, Weijun; Jones, Tim; Drake, Nick; Ignatyev, Konstantin; Davidson, Nicholas; Shi, Zongbo
发表日期2022
ISSN1680-7316
EISSN1680-7324
起始页码6045
结束页码6066
卷号22期号:9页码:22
英文摘要Mineral dust is the largest source of aerosol iron (Fe) to the offshore global ocean, but acidic processing of coal fly ash (CFA) in the atmosphere could be an important source of soluble aerosol Fe. Here, we determined the Fe speciation and dissolution kinetics of CFA from Aberthaw (United Kingdom), Krakow (Poland), and Shandong (China) in solutions which simulate atmospheric acidic processing. In CFA PM10 fractions, 8 %-21.5 % of the total Fe was found to be hematite and goethite (dithionite-extracted Fe), and 2%-6.5 % was found to be amorphous Fe (ascorbate-extracted Fe), while magnetite (oxalate-extracted Fe) varied from 3 %-22 %. The remaining 50 %-87 % of Fe was associated with other Fe-bearing phases, possibly aluminosilicates. High concentrations of ammonium sulfate ((NH4)(2)SO4), often found in wet aerosols, increased Fe solubility of CFA up to 7 times at low pH (2-3). The oxalate effect on the Fe dissolution rates at pH 2 varied considerably, depending on the samples, from no impact for Shandong ash to doubled dissolution for Krakow ash. However, this enhancement was suppressed in the presence of high concentrations of (NH4)(2)SO4. Dissolution of highly reactive (amorphous) Fe was insufficient to explain the high Fe solubility at low pH in CFA, and the modelled dissolution kinetics suggest that other Fe-bearing phases such as magnetite may also dissolve relatively rapidly under acidic conditions. Overall, Fe in CFA dissolved up to 7 times faster than in a Saharan dust precursor sample at pH 2. Based on these laboratory data, we developed a new scheme for the proton- and oxalate-promoted Fe dissolution of CFA, which was implemented into the global atmospheric chemical transport model IMPACT (Integrated Massively Parallel Atmospheric Chemical Transport). The revised model showed a better agreement with observations of Fe solubility in aerosol particles over the Bay of Bengal, due to the initial rapid release of Fe and the suppression of the oxalate-promoted dissolution at low pH. The improved model enabled us to predict sensitivity to a more dynamic range of pH changes, particularly between anthropogenic combustion and biomass burning aerosols.
学科领域Environmental Sciences; Meteorology & Atmospheric Sciences
语种英语
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号WOS:000792361400001
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/273527
作者单位University of Birmingham; Japan Agency for Marine-Earth Science & Technology (JAMSTEC); University of Haifa; University of Leeds; Zhejiang University; Cardiff University; University of London; King's College London; Diamond Light Source
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Baldo, Clarissa,Ito, Akinori,Krom, Michael D.,et al. Iron from coal combustion particles dissolves much faster than mineral dust under simulated atmospheric acidic conditions[J],2022,22(9):22.
APA Baldo, Clarissa.,Ito, Akinori.,Krom, Michael D..,Li, Weijun.,Jones, Tim.,...&Shi, Zongbo.(2022).Iron from coal combustion particles dissolves much faster than mineral dust under simulated atmospheric acidic conditions.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(9),22.
MLA Baldo, Clarissa,et al."Iron from coal combustion particles dissolves much faster than mineral dust under simulated atmospheric acidic conditions".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.9(2022):22.
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