Morphological and chemical classification of fine particles over the Yellow Sea during spring, 2015–2018

Kwak, Nohhyeon; Lee, Haebum; Maeng, Hyunok; Seo, Arom; Lee, Kwangyul; Kim, Seojeong; Lee, Meehye; Wan, Joo; Shin, B.; Park, Kihong

doi:10.1016/j.envpol.2022.119286

Cited by 6 publications

(6 citation statements)

References 38 publications

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“…Similar internal mixing particles between mineral dust and SSA have been found not only in the Pacific Ocean, but also in other regions (Okada et al, 1990;Niimura et al, 1998;Wagner et al, 2008;Kandler et al, 2017;Adachi et al, 2020;Kwak et al, 2022;Knopf et al, 2022). It is considered that the internal mixing of mineral dust and sea salt is formed by cloud processes (Niimura et al, 1998;Formenti et al, 2011).…”

Section: Single-particle Analysissupporting

confidence: 54%

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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Section: Single-particle Analysissupporting

confidence: 54%

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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“…In general, aging processes move the aerosol population toward a more internally mixed state (Riemer et al., 2019). However, despite the fact that the Yellow Sea is a sea, there were various types of aerosols over the Yellow Sea, and a significant portion of them was fresh aerosols that have not yet been internally mixed (Kwak et al., 2022). It is thought that this is because the distance from the pollutant source is not far, so the atmosphere over the Yellow Sea is greatly affected by the aerosols directly emitted from the pollutant sources.…”

Section: Resultsmentioning

confidence: 99%

A New CCN Number Concentration Prediction Method Based on Multiple Linear Regression and Non‐Negative Matrix Factorization: 1. Development, Validation, and Comparison Using the Measurement Data Over the Korean Peninsula

Park,

Yum,

Seo

et al. 2023

JGR Atmospheres

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To reduce uncertainty in climate change prediction, a large amount of cloud condensation nuclei number concentration (NCCN) data must be obtained. This study aimed to develop a new NCCN prediction method, hereafter MLRNMF method, that applies multiple linear regression (MLR) and non‐negative matrix factorization (NMF) to aerosol number size distribution data measured in Seoul and over the Yellow Sea. To verify the reliability of the MLRNMF method, a data set separated from the training data set was used, and sufficient time differences of several years were given between the two data sets to make them as independent as possible from each other. The predicted NCCN was in acceptable agreement with the measured NCCN. The coefficient of determination (R2) values between measured and predicted NCCN for the Yellow Sea and Seoul were 0.81 and 0.71, respectively. Mean fractional bias (MFB) and mean fractional error (MFE) also met the performance goals (<±30% and <+50%, respectively). The MLRNMF method had similar accuracy to the backward integration method but showed strength in robustness and the capability to take into account external mixing. The NCCN prediction methods trained using data of a specific season tended to underestimate/overestimate somewhat, but MFB and MFE for all four seasons met the performance goals except for MFB in using June–August (JJA) data, implying that the MLRNMF method trained using only the data of a specific season can predict NCCN for all four seasons to some extent. It is expected that abundant NCCN data can be obtained through the MLRNMF method in future studies.

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“…The own ship emissions can be identified using various measures, for example, high CO, NOx concentrations (Sun et al, 2020b), high BC concentrations (Alroe et al, 2019;Shank et al, 2012), regular cooking emissions (Cai et al, 2020), and wind speeds/directions between the ship stop and start operation (Ausmeel et al, 2020;Kwak et al, 2022). The contribution of ship Jiang et al, 2018;Karjalainen et al, 2022;Lack and Corbett, 2012;Wu et al, 2021;.…”

Section: Analyses Of Single Particlesmentioning

confidence: 99%

“…The BC outflows from Asia to the Pacific Ocean exhibit seasonal variations and originate from anthropogenic and biomass-burning sources in China, Siberia, and Southeast Asia (Matsui et al, 2013). Ship-based BC and EC measurements reveal significant influence of continental transport on remote oceanic regions, including the Bay of Bengal (Kedia et al, 2012), Indian Ocean (Kompalli et al, 2021), Southern Indian Ocean and the Southern Ocean (Ueda et al, 2018), North Sea (Bencs et al, 2020), Antarctic (Chaubey et al, 2013;Schmale et al, 2019), North Pacific (Taketani et al, 2016;Xing et al, 2014), Arctic (Pankratova et al, 2021;Sharma et al, 2019), Northeast Atlantic (Fossum et al, 2022), the Yellow Sea (Kwak et al, 2022), and Western Pacific (Ma et al, 2022). However, to our knowledge, the BC mass concentrations have been found to vary significantly across different oceans and seasons, with levels from 3 to 2800 ng m -3 and being influenced by anthropogenic activities and seasonal factors.…”

Section: Introductionmentioning

confidence: 99%

Morphological and optical properties of carbonaceous aerosol particles from ship emissions and biomass burning during a summer cruise measurement in the South China Sea

Sun,

Zhang,

Liang

et al. 2023

Preprint

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Abstract. Carbonaceous aerosols constitute a crucial component of atmospheric marine aerosols, among which black carbon (BC) and brown carbon (BrC) are important contributors to light absorption and hence the positive climatic radiative forcing in the marine atmosphere. We conducted a month-long (May 05–June 09, 2021) onboard sample collections and online measurements of carbonaceous aerosols to characterize their morphological and optical properties during a ship cruise in the South China Sea (SCS), covering a marine region of 11.9–24.5° N and 111.1–118.2° E. Single particles were collected by a single particle sampler and offline analyses were performed to investigate the mixing state and morphology using a transmission electron microscope (TEM). Online measurements of BC in PM2.5 were made by a seven-wavelength aethalometer and organic carbon (OC)/elemental carbon (EC) mass concentrations were measured by a semi-online OC/EC analyzer. Single particle samples were classified into two modes: “stop” when the ship was anchored and “navigation” when the ship sailed at high speed. Feret diameters of the single particles during navigation and stop showed size distributions with the lognormal fitting peaks at 307 and 325 nm, respectively. The fresh (without coating) and aged BC particles (after removal of coating by the electron beams in TEM) showed comparable median fractal dimensions (1.65 vs 1.66), in contrast to their different median lacunarities (0.53 vs 0.59). The aged BC particles showed narrower Feret diameters (298–1980 nm) during navigation than those (304–2982 nm) of freshly-emitted BC from the own ship during stop. Moreover, tar balls, as one important component of single particles from ship emissions and as the tracer of biomass burning, were identified with geometrical diameters of 160–420 nm in the TEM images. The energy dispersive X-ray spectroscopy (EDS) analyses showed those tar balls are mainly mixed with sea salt, organics, BC, and sulfate. We also found a significant fraction of aged BC in various mixing states (core-shell, embedded) with other components of the aerosol particles after long-range transport. The campaign was further divided into several periods (before monsoon period, BMP; transition monsoon period, TMP; after monsoon period, AMP; and ship pollution period, SPP) according to the wind direction during monsoon and the own ship pollution. The median OC/EC ratios were 8.14, 5.20, 6.35, and 2.63 during BMP, TMP, AMP, and SPP, respectively, showing higher OC/EC ratios for biomass burning emissions than for fossil fuel emissions. Additionally, the median absorption Angström exponent (AAE) values derived from all wavelengths were 1.14, 1.02, 1.08, and 1.06 for BMP, TMP, AMP and SPP, respectively. Particularly, a median AAE value of 1.93 was obtained during two significant biomass burning events. These results showed that biomass burning (BB) and fossil fuel (FF) combustion contributed to 18–22 % and 78–82 % of all the BC light absorption without the two intense biomass burning events, during which BB and FF accounted for 42 % and 58 %, respectively. The two BB events originated from the Philippines and Southeast Asia before and after the summer monsoon. Our results demonstrated that BC can serve as the core of aged particles but the fractal dimensions of BC aggerates were subject to little variation; moreover, such BC particles become much more aggerated after aging in the marine atmosphere, which further affects the light absorption of the BC particles in the SCS. This study provides information about the morphology and the optical properties of carbonaceous aerosols which can be used to evaluate their effects on light absorption and hence the climatic radiative forcing in the SCS region.

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Morphological and chemical classification of fine particles over the Yellow Sea during spring, 2015–2018

Cited by 6 publications

References 38 publications

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

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

A New CCN Number Concentration Prediction Method Based on Multiple Linear Regression and Non‐Negative Matrix Factorization: 1. Development, Validation, and Comparison Using the Measurement Data Over the Korean Peninsula

Morphological and optical properties of carbonaceous aerosol particles from ship emissions and biomass burning during a summer cruise measurement in the South China Sea

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