Determination of calcium and sulfate species in aerosols associated with the conversion of its species through reaction processes in the atmosphere and its influence on cloud condensation nuclei activation

Miyamoto, Chihiro; Yamakawa, Yoshiaki; Takahashi, Yoshio

doi:10.1016/j.atmosenv.2019.117193

Cited by 11 publications

(13 citation statements)

References 35 publications

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“…The aerosols were separated into seven size fractions using the cascade impactor (Stage ], <0.39 µm). Details of the samples were described in our previous studies [7,20].…”

Section: Methodsmentioning

confidence: 99%

“…For comparison, Ca speciation was also conducted by Ca K-edge XANES measured at BL-9A at the Photon Factory (Tsukuba, Japan). Details of the Ca K-edge XANES were identical to those reported in our previous studies [1,7]. Linear combination fitting (LCF) of each spectrum by endmembers of possible Mg or Ca species and principal component analysis (PCA) to obtain the number of endmembers needed for the LCF were conducted using Athena software [21].…”

Section: Methodsmentioning

confidence: 99%

“…This mineral is an important component in aerosols because it is reactive with acidic species such as sulfuric acid, nitric acid, and organic acids in the atmosphere [3][4][5]. As a result, Ca in aerosols can mitigate acid deposition through the neutralization of acidic species, which produces Ca nitrate, Ca sulfate, and Ca oxalate in aerosols [2,6,7]. Meanwhile, many studies have assumed that most Mg in the atmosphere is present as Mg carbonate (e.g., dolomite and magnesite) in aerosols [5,8], which can also react with acidic species.…”

Section: Introductionmentioning

confidence: 99%

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Speciation of Magnesium in Aerosols Using X-ray Absorption Near-Edge Structure Related to Its Contribution to Neutralization Reactions in the Atmosphere

2021

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Aerosols, including mineral dust, are transported from China and Mongolia to Japan, particularly in spring. It has been recognized that calcium (Ca) carbonate is the main Ca species in aerosols, which reacts with acidic species such as sulfuric and nitric acids at the surface of mineral dust during its long-range transport, related to mitigation of acid depositions. The similar assumption that magnesium (Mg) originally takes the form of carbonate and contributes to the neutralization reaction and buffering effect on the acidity of aerosols has been suggested in various studies. However, few studies have confirmed this process by measuring actual Mg species in aerosols quantitatively. In this study, X-ray absorption near-edge structure (XANES) spectroscopy was employed to determine Mg species in size-fractionated aerosol samples, including mineral dust. The results showed that (i) most Mg in the mineral dust did not take the form of carbonate and its reacted species (e.g., sulfate and nitrate) produced by the neutralization reaction, but (ii) Mg was mainly found as Mg in the octahedral layer in phyllosilicates. Given that the reactivity of such Mg in phyllosilicates is much lower than those in carbonate minerals, the contribution of Mg to the neutralization reactions in the atmosphere must be lower than previously expected.

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“…The aerosols were separated into seven size fractions using the cascade impactor (Stage ], <0.39 µm). Details of the samples were described in our previous studies [7,20].…”

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Speciation of Magnesium in Aerosols Using X-ray Absorption Near-Edge Structure Related to Its Contribution to Neutralization Reactions in the Atmosphere

2021

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“…S3d) indicated that non-SSA-NO3 − was present in coarse aerosol particles in the form of Ca(NO3)2. However, our previous study identified gypsum (CaSO4•2H2O) rather than Ca(NO3)2 as the dominant secondary Ca species in coarse aerosol particles collected in January, November, and the Asian dust event (Miyamoto et al, 2020). Recent studies have demonstrated that hygroscopic Ca(NO3)2 on the surfaces of mineral dust reacted with (NH₄)₂SO₄, resulting in the formation of NH4NO3 and CaSO4•2H2O (Wu et al, 2019(Wu et al, , 2020.…”

Section: Anionsmentioning

confidence: 97%

Measurement report: Stoichiometry of dissolved iron and aluminum as an indicator of the factors controlling the fractional solubility of aerosol iron: Results of the annual observations of size-fractionated aerosol particles in Japan

Sakaguchi

Yamakawa

Miyamoto

et al. 2023

Preprint

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Abstract. Atmospheric deposition of iron (Fe) in aerosol particles is enhanced primary production on the ocean surface, resulting in promoting the uptake of carbon dioxide into the surface seawater. Atmospheric deposition of iron (Fe) promotes primary production in the surface ocean, resulting in enhanced uptake of carbon dioxide into surface seawater. Since microorganisms in seawater utilize dissolved Fe (d-Fe) as a nutrient, the bioavailability of Fe in aerosol particles depends on its solubility. However, factors controlling fractional Fe solubility (Fesol%) in aerosol particles have not been fully understood. This study performed annual observations of Fesol% in size-fractionated (seven fractions) aerosol particles at Higashi-Hiroshima, Japan. In particular, the feasibility of the molar concentration ratio of d-Fe relative to dissolved Al ([d-Fe]/[d-Al]) as an indicator of the sources of d-Fe in aerosol particles because this ratio is likely dependent on the emission sources of Fe (e.g., mineral dust, fly ash, and anthropogenic Fe oxides) and their dissolution processes (proton-promoted and ligand-promoted dissolutions). Approximately 70 % of total Fe and dissolved Fe was present in coarse and fine aerosol particles, respectively, and the average Fesol% in fine aerosol particles (11.4 ± 6.97 %) was higher than that of coarse aerosol particles (2.19 ± 2.27 %). In addition, the average ratio of [d-Fe]/[d-Al] in coarse aerosol particles (0.408 ± 0.168) was lower than that in fine aerosol particles (1.15 ± 0.803). The range of [d-Fe]/[d-Al] ratios in the coarse aerosol particles (0.121–0.927) was similar to that obtained by proton-promoted dissolutions of mineral dust (0.1–1.0), indicating that d-Fe in coarse aerosol particles were derived from mineral dust. The [d-Fe]/[d-Al] ratios of aerosol particles ranged from 0.386 to 4.67, and [d-Fe]/[d-Al] ratios greater than 1.5 cannot be explained by proton-promoted dissolution and ligand-promoted dissolution (1.0 < [d-Fe]/[d-Al] < 1.5). The [d-Fe]/[d-Al] ratio correlated with the enrichment factor of Fe in fine aerosol particles (r: 0.505), indicating that anthropogenic Fe with a high [d-Fe]/[d-Al] ratio was the source of d-Fe in fine aerosol particles. The high [d-Fe]/[d-Al] ratio was attributed to Fe-oxides emitted from high-temperature combustions (high-temp-FeOx). Finally, the fraction of high-temp-FeOx to d-Fe in total suspended particulate (TSP) was calculated based on the [d-Fe]/[d-Al] ratio of aerosols and their emission source samples. As a result, the fraction of high-temp-FeOx to d-Fe in TSP varied from 1.48 to 80.7 %. The high fraction was found in summer when air masses originated from industrial regions in Japan. By contrast, approximately 10 % of d-Fe in the TSP samples collected in spring and during Asian dust events was derived from high-temp-FeOx, when air masses were frequently transported from East Asia to the Pacific Ocean. Thus, mineral dust is the dominant source of d-Fe in Asian outflow to the Pacific Ocean.

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“…In this study, the buffering effect of calcite in the equilibrium calculation was not considered because (i) mineral dust was likely acidified beyond the buffering capacity of calcite, and (ii) calcite in fine aerosol particles was altered to CaSO 4 q 2H 2 O and CaC 2 O 4 during transport from the source region of Asian dust to Japan (Takahashi et al, 2008;Miyamoto et al, 2020).…”

Section: Geochemical Modeling Of L-fe Speciesmentioning

confidence: 99%

Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility

et al. 2022

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Abstract. Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fesol%) in marine aerosol particles. However, the impact of these processes on Fesol% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fesol% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fesol% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fesol% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM>1.3) and fine aerosol particles (PM1.3). Approximately 80 % of the total Fe (insoluble + labile Fe) was present in PM>1.3, whereas labile Fe was mainly present in PM1.3. The Fesol% in PM>1.3 was not significantly increased (2.56±2.53 %, 0.00 %–8.50 %, n=20) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM1.3 was acidified beyond the buffer capacity of calcite. As a result, Fesol% in PM1.3 (0.202 %–64.7 %, n=10) was an order of magnitude higher than that in PM>1.3. The PM1.3 contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fesol%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM1.3 established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH < 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.

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Determination of calcium and sulfate species in aerosols associated with the conversion of its species through reaction processes in the atmosphere and its influence on cloud condensation nuclei activation

Cited by 11 publications

References 35 publications

Speciation of Magnesium in Aerosols Using X-ray Absorption Near-Edge Structure Related to Its Contribution to Neutralization Reactions in the Atmosphere

Speciation of Magnesium in Aerosols Using X-ray Absorption Near-Edge Structure Related to Its Contribution to Neutralization Reactions in the Atmosphere

Measurement report: Stoichiometry of dissolved iron and aluminum as an indicator of the factors controlling the fractional solubility of aerosol iron: Results of the annual observations of size-fractionated aerosol particles in Japan

Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility

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