Observation of transformation of calcite to gypsum in mineral aerosols by Ca K-edge X-ray absorption near-edge structure (XANES)

Takahashi, Yoshio; Miyoshi, Takuro; Yabuki, Sadayo; Inada, Yuji; Shimizu, Hiroshi

doi:10.1016/j.atmosenv.2008.04.012

Cited by 39 publications

(53 citation statements)

References 25 publications

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“…Calcite is the most abundant mineral found over the northwestern arid regions surrounded by the Arabian Sea. These calcite crystals will get lifted with dust particles and undergo reaction with atmospheric sulfate to produce calcium sulfate (i.e., gypsum) (Takahashi et al 2008). Mori et al (1998) found that ammonium sulfate reacted with calcium carbonate in Kosa (Asian dust) particles.…”

Section: Resultsmentioning

confidence: 99%

Organic and inorganic components of aerosols over the central Himalayas: winter and summer variations in stable carbon and nitrogen isotopic composition

Hegde

Kawamura

Joshi

et al. 2015

Environ Sci Pollut Res

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The aerosol samples were collected from a high elevation mountain site, Nainital, in India (1958 m asl) during September 2006 to June 2007 and were analyzed for water-soluble inorganic species, total carbon, nitrogen, and their isotopic composition (δ(13)C and δ(15)N, respectively). The chemical and isotopic composition of aerosols revealed significant anthropogenic influence over this remote free-troposphere site. The amount of total carbon and nitrogen and their isotopic composition suggest a considerable contribution of biomass burning to the aerosols during winter. On the other hand, fossil fuel combustion sources are found to be dominant during summer. The carbon aerosol in winter is characterized by greater isotope ratios (av. -24.0‰), mostly originated from biomass burning of C4 plants. On the contrary, the aerosols in summer showed smaller δ(13)C values (-26.0‰), indicating that they are originated from vascular plants (mostly of C3 plants). The secondary ions (i.e., SO4 (2-), NH4 (+), and NO3 (-)) were abundant due to the atmospheric reactions during long-range transport in both seasons. The water-soluble organic and inorganic compositions revealed that they are aged in winter but comparatively fresh in summer. This study validates that the pollutants generated from far distant sources could reach high altitudes over the Himalayan region under favorable meteorological conditions.

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Section: Resultsmentioning

confidence: 99%

Organic and inorganic components of aerosols over the central Himalayas: winter and summer variations in stable carbon and nitrogen isotopic composition

Hegde

Kawamura

Joshi

et al. 2015

Environ Sci Pollut Res

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“…The helium flow rate was set at 20 mL/min. SF 6 gas exiting the columns was frozen into two glass traps and was subsequently transferred to a sample bellows of a dual inlet ThermoFinnigan MAT 253 mass spectrometer where purified SF 6 [Quan et al, 2008;Takahashi et al, 2008]. But in a heavily populated and industrialized region such as Beijing, coal combustion seems a likely source.…”

Section: Isotopic Analysis Of Sulfur Isotopesmentioning

confidence: 99%

Identification of sources and formation processes of atmospheric sulfate by sulfur isotope and scanning electron microscope measurements

et al. 2010

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[1] Atmospheric sulfate aerosols have a cooling effect on the Earth's surface and can change cloud microphysics and precipitation. China has heavy loading of sulfate, but their sources and formation processes remain uncertain. In this study we characterize possible sources and formation processes of atmospheric sulfate by analyzing sulfur isotope abundances ( 32 S, 33 S, 34 S, and 36 S) and by detailed X-ray diffraction and scanning electron microscope (SEM) imaging of aerosol samples acquired at a rural site in northern China from March to August 2005. The comparison of SEM images from coal fly ash and the atmospheric aerosols suggests that direct emission from coal combustion is a substantial source of primary atmospheric sulfate in the form of CaSO 4 . Airborne gypsum (CaSO 4 ·2H 2 O) is usually attributed to eolian dust or atmospheric reactions with H 2 SO 4 . SEM imaging also reveals mineral particles with soot aggregates adhered to the surface where they could decrease the single scattering albedo of these aerosols. In summer months, heterogeneous oxidation of SO 2 , derived from coal combustion, appears to be the dominant source of atmospheric sulfate. Our analyses of aerosol sulfate show a seasonal variation in D 33 S (D 33 S describes either a 33 S excess or depletion relative to that predicted from consideration of classical mass-dependent isotope effects). Similar sulfur isotope variations have been observed in other atmospheric samples and in (homogenous) gas-phase reactions. On the basis of atmospheric sounding and satellite data as well as a possible relationship between D 33 S and Convective Available Potential Energy (CAPE) during the sampling period, we attribute the sulfur isotope anomalies (D 33 S and D 36 S) in Xianghe aerosol sulfates to another atmospheric source (upper troposphere or lower stratosphere).Citation: Guo, Z., Z. Li, J. Farquhar, A. J. Kaufman, N. Wu, C. Li, R. R. Dickerson, and P. Wang (2010), Identification of sources and formation processes of atmospheric sulfate by sulfur isotope and scanning electron microscope measurements,

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“…The analysis depth, rather than the probing depth, for FY-mode, which is free from the thickness effect that can attenuate peaks in XANES spectra, 14 can be practically larger than the aerosol particle size examined here, because identical spectra between FY-and CEY-modes for unreacted calcite particles were obtained in the previous study (particle size 4.77.0¯m). 10 Hence, the combination of FY-and CEY-modes makes it possible to determine Ca species in the whole and at the surface of each particle. 9,10 XANES spectra obtained were fitted by a linear combination of spectra of reference materials as reported in Takahashi et al 10 to estimate mole ratios of Ca species present in individual particles.…”

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confidence: 99%

“…10 Hence, the combination of FY-and CEY-modes makes it possible to determine Ca species in the whole and at the surface of each particle. 9,10 XANES spectra obtained were fitted by a linear combination of spectra of reference materials as reported in Takahashi et al 10 to estimate mole ratios of Ca species present in individual particles. The least-squares fitting of the spectra was conducted using REX2000 (Rigaku Co., Tokyo, Japan).…”

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confidence: 99%

“…9 They analyzed samples collected in Aksu (near the Taklimakan Desert), Qingdao (urban area in eastern China), and Tsukuba (eastern Japan) during a large dust event in March, 2002, using sulfur (S) and Ca speciation by S and Ca K-edge X-ray absorption near-edge structure (XANES) spectroscopy, or the structure near absorption edge in X-ray absorption fine structure (XAFS). 10 The main Ca species determined by the spectra were calcite (CaCO 3 ) and gypsum (CaSO 4 ¢2H 2 O) and the mole ratio of gypsum to total Ca (= measured by ion chromatography) were estimated. The gypsum fraction, which is a neutralization product, relative to total Ca for the bulk analysis increased in the order from Aksu, Qingdao to Tsukuba.…”

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confidence: 99%

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Depth-dependent Calcium Speciation in Individual Aerosol Particles by Combination of Fluorescence Yield and Conversion Electron Yield XAFS Using X-ray Microbeam

Miyamoto¹,

Marcus²,

Kurisu³

et al. 2016

Chem. Lett.

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Observation of transformation of calcite to gypsum in mineral aerosols by Ca K-edge X-ray absorption near-edge structure (XANES)

Cited by 39 publications

References 25 publications

Organic and inorganic components of aerosols over the central Himalayas: winter and summer variations in stable carbon and nitrogen isotopic composition

Organic and inorganic components of aerosols over the central Himalayas: winter and summer variations in stable carbon and nitrogen isotopic composition

Identification of sources and formation processes of atmospheric sulfate by sulfur isotope and scanning electron microscope measurements

Depth-dependent Calcium Speciation in Individual Aerosol Particles by Combination of Fluorescence Yield and Conversion Electron Yield XAFS Using X-ray Microbeam

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