Atmospheric Environment 317 (2024) 120201

Contents lists available at ScienceDirect

Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

Latitudinal distribution and sources analysis of greenhouse gases and air

pollutants observed during the 2021 Yellow Sea Air Quality campaign
aboard a research vessel
Shanlan Li a, *, Samuel Takele Kenea a, Sumin Kim a, Hee-Jung Yoo a, Sangwon Joo a,
Haeyoung Lee a, b, Sangmin Oh a, Min Jae Jeong a, Wonick Seo a, Miyoung Ko a, Soojeong Lee a,
Young-Suk Oh a, Daegeun Shin a
a
Climate Research Department, National Institute of Meteorological Sciences, Seogwipo-si, Jeju-do, 63568, Republic of Korea
b
Tropospheric Chemistry, National Institute of Water and Atmospheric Research, Te Whanganui-a-Tara/Wellington, 6011, New Zealand

H I G H L I G H T S

• Yellow Sea Air Quality campaign studies greenhouse/air pollutants distribution.

• Greenhouse/air pollutants show a clear latitudinal gradient over Yellow Sea.
• CO, CO2, CH4 correlation suggests fossil fuel-based sources mainly from China and Korea.
• Highly elevated CH4 linked to microbial-related biogenic emissions from Korean based on STILT analysis.

A R T I C L E I N F O A B S T R A C T

Keywords: The Yellow Sea serves as a pathway for air pollution transport from the Asian continent into Korea and is
Research vessel annually monitored by the Korean Meteorological Administration (KMA) research vessel during the spring
Yellow sea season. This study investigated the spatio-temporal variation of long-range transported greenhouse gases (CO2
YES-AQ campaign
and CH4) and air pollutants (CO, NOx, SO2, O3) in the Yellow Sea during the Yellow Sea Air Quality (YES-AQ)
GHGs
campaign. Our analysis reveals that GHGs and air pollutants exhibit a clear latitudinal distribution. Lower
Air pollutants
Correlation analysis concentrations are observed in the range of 31.2–34.5◦ N, primarily influenced by air masses traversing the ocean
and the western part of Korean Peninsula. In contrast, higher concentrations occur more frequently at
34.5–37.8◦ N, primarily affected by continental air masses. The regression slopes of CO and CO2 vary depending
on regional characteristics, particularly in air originating from Korea and China. Regression slope analysis be­
tween CO, CO2, and CH4, except for high plume of CH4 (>2.05 ppm), indicates that fossil fuel sources play a
significant role. A high plume of CH4 (>2.05 ppm) was observed on April 22nd, coinciding with the maximum O3
concentrations during the period of highest temperatures throughout the voyage. The potential source regions
were identified in the west-southern coast of Korea, using footprint analysis from Stochastic Time-Inverted
Lagrangian Transport (STILT) and column-averaged dry-air mole fraction of CH4 (XCH4) retrieval from the
TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor (S5P) satellite. The high
CH4 enhancements are most likely due to biogenic emissions triggered by favorable near-surface temperatures
for microbial activities in soil. Furthermore, the high CH4 enhancements were not correlated with CO and CO2,
indicating that the source was not related to fossil fuel combustion. On March 29–30, a high plume of NOx was
detected and is likely attributed to the Bohai Sea, which is located just above the Yellow Sea and surrounded by
highly industrialized and semi-enclosed areas.

* Corresponding author.
E-mail addresses: sunranlee@korea.kr, sunranlee18@gmail.com (S. Li).

https://doi.org/10.1016/j.atmosenv.2023.120201
Received 28 April 2023; Received in revised form 1 November 2023; Accepted 6 November 2023
Available online 14 November 2023
1352-2310/© 2023 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
S. Li et al.
1. Introduction
East Asia is one of the major source regions of anthropogenic trace
gases, and their emissions have been rapidly increasing due to recent
economic growth in the region (Crawford et al., 2021; Labzovskii et al.,
2019). Due to China’s rapid economic growth in recent years, its relative
contribution to emissions in Asia has been the largest. In fact, China has
become the largest anthropogenic CO2 emitter in the world, surpassing
the United States (Gregg et al., 2008; Peters et al., 2012). However, the
emissions of SO2 in Asia have declined significantly, especially in China,
with a 10% reduction from 2005 to 2010 as a result of improvements in
flue gas desulfurization installations (Sun et al., 2018). NOx emissions
stopped rising and started falling in 2011 with the introduction of new
technologies in China, such as selective catalytic reduction in large
power plants and regulations for road vehicles (Jiang et al., 2022;
Kurokawa and Ohara, 2020; Zheng et al., 2018a), although NOx emis­
sions from China accounted for about 20% of global emissions in 2018
(Crippa et al., 2022). Surface ozone also shows an increasing trend,
especially in megacities in East Asia, despite the significant reduction of
NOx, which could also affect the enhanced O3 concentrations
throughout the Asia-Pacific region via long-range transport because the
surface O3 does not respond to linear reductions in NOx (Lee et al., 2020,
2021). The Yellow Sea serves as an ideal monitoring location for the
inflow of Asian pollution towards Korea, Japan, and the Western Pacific
region, given its strategic location on the downwind side of the westerly
wind direction. Nonetheless, studies on the importance of observations
in the Yellow Sea and the continuous collection of air pollution and GHG
data in the region are lacking.
The Korean Meteorological Administration (KMA) has routinely
performed in-situ observations of main GHGs such as CO2 and CH4
(Kenea et al., 2021, 2023a; Lee et al., 2019) and air pollutants such as
CO, SO2, NOx, and O3 at the Anmyeon-do (AMY) and Jeju Gosan (GSN)
stations (Li et al., 2022) for several decades, which are the World
Meteorological Organization/Global Atmospheric Watch (WMO/GAW)
regional background stations in South Korea. Additionally, the research
vessel has established and conducted a special campaign every spring to
diagnose air pollution, especially for long-range transported pollutants
via the Yellow Sea (Jeong et al., 2022; Kim et al., 2022; Shin et al.,
2022). The first aerosol samples collected by the KMA research vessel
over the Yellow Sea in 2015 were dominated by secondary ionic species
2-
such as NH+ 4 , nss-SO4 , and NO3 in PM10 and PM2.5, suggesting that PM10
−
(PM2.5) was affected by mobile (stationary) sources (Cha et al., 2020; Ko
et al., 2017). Since 2018, the KMA has adapted the research aircraft
(King Air 350) to design an air quality monitoring campaign over the
Yellow Sea (YES-AQ: Yellow Sea Air Quality) by integrating surface
in-situ, vessel, and aircraft measurements during the spring season when
frequent haze events occur over the Asia-Pacific (Jeong et al., 2022). In
March 2021, an extremely high Asian dust event occurred in China and
the Korean region and the research vessel first detected high levels of
PM10 (Kim et al., 2022). The KMA issued an Asian dust warning for the
first time in five years due to PM10 concentrations exceeding 800 μg/m3.
A combination of aircraft and vessel observations can help understand
the physical and chemical properties of PM and gaseous pollutants in the
upper and lower troposphere (Kim et al., 2022). In particular, the
analysis of simultaneous observation data from surface stations, satel­
lites, and aircrafts using inter-species correlation slopes, enabled the
detection of the occurrence of the stratification of atmospheric pollution
plumes containing CO and PM in the troposphere (Li et al., 2022).
The prevailing winds over the Yellow Sea in spring exhibit westerly
or easterly patterns, resulting in frequent measurements of air outflow
from the Asian continent. This region also serves as a pathway for the
transport of air pollutants into Korea. The purpose of the YES-AQ
campaign is to precisely analyze the characteristics of air pollution,
greenhouse gases, and Asian dust flowing into the Yellow Sea from the
Asian continent. This study analyzed greenhouse gases such as CO2 and
CH4, and air pollutants such as CO, O3, SO2, and NOx observed in the
2
Atmospheric Environment 317 (2024) 120201
Yellow Sea during March–April 2021. We used the total column amount
of NO2 and column-averaged dry-air mole fraction of CH4 (XCH4) from
the TROPOspheric Monitoring Instrument (TROPOMI) onboard the
Sentinel-5 Precursor (S5P) (Landgraf et al., 2016) satellite and Korean
Integrated Model (KIM) (Hong et al., 2018) - Stochastic Time-Inverted
Lagrangian Transport (STILT) (Fasoli et al., 2018) footprint sensitivity
to identify the predominant pollution source regions for highly elevated
gaseous events observed from the vessel. The findings of this study
provide insights into pollution transport over the Yellow Sea, facilitating
the identification of emissions sources and addressing transboundary air
pollution issues in East Asia. This paper is structured as follows: Section
2 provides a concise introduction to the YES-AQ campaign; Section 3
presents a brief overview of the data and methodology employed in this
study; and Section 4 presents the results and discussion, followed by the
conclusion in Section 5.
2. YES-AQ campaign overview
The YES-AQ campaign has been conducted annually during the
spring season (March–May) since 2018 over the Yellow Sea. The Yellow
Sea is not only influenced by emissions from both Korea and China but
also serves as a monitoring location for the inflow of Asian pollution
towards Korea, Japan, and the Western Pacific region owing to its
strategic location on the downwind side of the westerly wind direction.
The GAW regional background stations, such as AMY located on the
northwest coast of Korea at 36.53◦ N, 126.32◦ E, and GSN located on the
southwest coast of Korea at 33.29◦ N, 126.16◦ E, are also situated on the
downwind side of the westerly wind direction. However, it is essential to
consider the surrounding emission sources when interpreting observa­
tions from these surface stations (Li et al., 2022). Nonetheless, studies on
the importance of the observations in the Yellow Sea and the continuous
collection of air pollution and GHG data in the region are lacking. To
address this gap, the KMA has taken the initiative to establish the
infrastructure of the Gisang 1 Research vessel for ongoing monitoring.
The primary aim of this effort is to better comprehend the transboundary
transport of pollution from the Asian continent. Since 2018, the
campaign has been organized by the KMA/National Institute of Meteo­
rological Sciences (NIMS) along with several universities and research
institutes, each contributing with distinct scientific objectives (Jeong
et al., 2022; Kim et al., 2022; Park et al., 2021; Shin et al., 2022; You
et al., 2021). The main objective of the campaign is to enhance our
understanding of the air pollutants over the Yellow Sea, leveraging in­
tegrated surface in-situ stations, research vessels, and aircraft for
comprehensive analysis using onboard payloads (Li et al., 2020, 2022;
Table S1).
3. Data and methodology
3.1. Vessel observation
Research vessel Gisang 1 (Fig. S1) is a 498-ton weather observation
ship operated by the KMA/NIMS and has been in operation since 2011 to
conduct three-dimensional weather observations over the ocean. The
ship conducts observations for marine meteorology, upper-level mete­
orology, and ocean physics aboard observations and is operated for
more than 160 days per year, covering the Yellow Sea, South Sea, and
coastal areas of Korea. However, the intensive air quality campaign on
the vessel started in 2017 with the establishment of the King Air research
aircraft platform. Subsequently, the YES-AQ campaign was carried out
annually during the spring (Kim et al., 2022; Park et al., 2018, 2021;
Shin et al., 2022). The objective of the campaign is to investigate
long-range transported air pollutants over the Yellow Sea, leveraging
integrated surface in-situ stations, research vessels, and aircraft for
comprehensive analysis.
The research vessel was equipped with multiple instruments to
measure various compositions, including the mass concentration of PM,
S. Li et al.
aerosol size distribution, aerosol absorption coefficients, water-soluble
ion components, GHGs such as CO2 and CH4, and air pollutants such
as CO, NOx, SO2, and O3. All measurements were conducted in an air-
conditioned container, and sample inlets (for CO2, CH4, and CO) were
located at the topmost platform of the bow (10 m above mean sea level)
away from local sources on the vessel (chimney stacks towards the
stern). Air samples were pumped using a KNF diaphragm pump (7 bar)
through a 50 m de-carbon tube (10 mm) at approximate heights of 10 m
above sea level. The sampled air was dried using a cryogenic method
(CT-90, Operon, Korea). The drying system consisted of two chambers
with sequential cooling steps. The ambient air was first cooled to − 20 ◦ C
in the first chamber and then further cooled to − 50 ◦ C in the second
chamber. This drying system has also been installed at several regional
background stations in Korea, such as AMY, GSN, and Ulleungdo (ULD).
For more detailed information, refer to Lee et al. (2019, 2023). An inlet
for more reactive gases such as O3, NOx, SO2, and aerosols was installed
on the roof of the measurement container (Fig. S1), located just above
the ship’s wheelhouse.
The research vessel has been conducting observations of several
compositions along the north-south direction of 31.2–37.8◦ N in the
Yellow Sea, as shown in Fig. 1. Typically, the daily mission starts early in
the morning (7:00 a.m. LST: UTC + 9) and ends around 5:00 p.m. (LST),
covering a south-north (or north-south) track of approximately 200 km
per day. However, night missions are also conducted, spanning from day
to night, when strong Asian dust is detected on 28–30th March 2021.
3.2. Data quality control
In this study, we focused on the main GHGs such as CO2 and CH4, as
well as air pollutants such as O3, CO, SO2, and NOx observed during the
2021 YES-AQ campaign. We did not include detailed observation
methods and results related to PM in this study, as more information can
be found in Kim et al. (2022) and Shin et al. (2022). The greenhouse gas
CO2 and CH4 measurements employed a commercial analyzer developed
by Picarro Inc. (Cavity Ring-Down Spectroscopy, CRDS, model G2301,
Santa Clara, CA). The CRDS measures CO2 and CH4 with high precision
using a laser beam entering an optical cavity cell with highly reflective
mirrors (optical path length of 15–20 km). This method utilizes a
high-precision wavelength monitor, as well as controlled pressure and
temperature within the measurement cell to achieve accurate mea­
surements of trace gases with high precision. CRDS is known for its
stability and drift-free nature over both short and long timescales
(Karion et al., 2013; Rella et al., 2013). CRDS instruments were
Fig. 1. (a) Accumulated track of the research vessel during the 2021 YES-AQ campaign, with stars representing the Anmyeon-do (AMY: 36.53◦ N, 126.32◦ E) and Jeju
Gosan (GSN: 33.29◦ N, 126.16◦ E) stations, which are regional background stations under the World Meteorological Organization/Global Atmosphere Watch (WMO/
GAW). (b) Enhanced CO2 dry mole fractions (ΔCO2: Observation over the Yellow Sea minus background level constrained from the AMY station on the same date)
along with typical tracks on March 29, 2021.
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Atmospheric Environment 317 (2024) 120201
calibrated before deployment using four laboratory standards that were
made in the NIMS calibration center in Jeju, Korea. Calibration scale
transfer was performed using CRDS and WMO GAW Central Calibration
Laboratory (CCL)-provided standard gases, which were traceable to the
WMO-X2019A scale for CO2 and WMO-X2004A scale for CH4, with
uncertainties of less than 0.2 ppm and 2 ppb, respectively. The scale
propagation uncertainty is described in Lee et al. (2019). To assess data
drift during the one-month campaign, we injected a working standard
once per day for 20 min, which was sampled at the AMY station and
certified by the central laboratory of the NIMS. We estimated the drift to
be 0.14 ppm for CO2 and 0.6 ppb for CH4 (Fig. S2), which is comparable
with the WMO/GAW compatibility goal. Reactive gases such as NOx,
SO2, O3, and CO were measured using a model 42i (NO–NO2-NOx)
analyzer, 43i SO2 analyzer, 48i CO analyzer, and 49i ozone analyzer,
respectively, developed by Thermo Scientific. All instruments were
calibrated with WMO scale standard gas in the laboratory before
deployment.
In this study, we applied the following criteria to exclude measure­
ment data.
1. Data recorded when the research vessel was in port or at rest.
2. Data during the drift check.
3. Data points with a relative wind direction measured on the vessel
(with the fixed reference point being the prow of the vessel) that
were outside the range 150–210◦ were excluded to exclude potential
contamination from onboard activities such as emissions from
chimney stacks.
The data classified according to these criteria are presented in
Fig. S3. A total of 46% of the data were excluded based on the first and
second criteria, and 0.8% of the data were excluded based on the third
criterion. Thus, 54.2% of the observational data were analyzed in this
study. During the 2021 YES-AQ campaign, the vessel sought shelter and
anchored at ports on several occasions due to adverse weather condi­
tions in the Yellow Sea. Socheongdo (37.75◦ N, 124.73◦ E) and Mokpo
(34.78◦ N, 126.38◦ E) harbors were selected as shelter positions in the
northern and southern parts, respectively. To mitigate the influence of
nearby port areas, observations collected during the vessel’s navigation
to these ports were omitted from the analysis. This study focused
exclusively on samples collected within the longitude range of 124◦ E to
125◦ E.
S. Li et al. Atmospheric Environment 317 (2024) 120201

3.3. TROPOMI/S5P satellite data
The TROPOMI/S5P satellite was launched on October 13, 2017, and
placed in a near-polar, Sun-synchronous orbit with a mean altitude of
824 km above the Earth’s surface. The equator crossing time was 1:30 p.
m. (LST: UTC+9), and the repeat cycle was 16 days (Landgraf et al.,
2016; Veefkind et al., 2012). TROPOMI/S5P has been continuously
providing global coverage of XCH4 daily since its launch in October
2017. The spatial resolution of measurements initially stood at 7 × 7
km2 and was further improved to 5.5 × 7 km2 in August 2019. In this
study, we utilized the SRON RemoTec-S5P XCH4 product, version 2.5.0,
which adheres closely to the mission’s requirements for precision and
accuracy, maintaining a level below 1% (Hasekamp et al., 2021).
Specifically, we employed bias-corrected estimates of XCH4 accompa­
nied by a quality assurance flag (QA) of 1. The bias-corrected XCH4
retrievals used in our analysis have been validated using the Total
Carbon Column Observing Network (TCCON), demonstrating their high
data quality (Lorente et al., 2021). We also utilized TROPOMI/S5P NO2
tropospheric total column amount data (version 1.4.0) with the rec­
ommended quality value (QA) of >0.75 (van Geffen et al., 2022). By
leveraging these datasets, we can examine the detailed spatial distri­
bution of significant CH4 and NO2 enhancements within the source
regions.

Fig. 2. Box chart with 1-σ standard deviations showing the average concentrations of (a) CO2, (b) CH4, (c) CO, (d) O3, (e) NOx, and (f) SO2 at a latitude of 0.05◦ bin
during the YES-AQ campaign. The blue and red lines with shading represent the monthly means and range of uncertainty of each composition observed at the
Anmyeon-do (AMY) and Jeju Gosan (GSN) surface stations, respectively.

4
S. Li et al.
3.4. Footprint sensitivity analysis based on back-trajectory
In this study, we utilized the single-particle Lagrangian model of
HYSPLIT (Stein et al., 2015) and the Particle dispersion model of STILT
(version 2, Fasoli et al., 2018), coupled with meteorological data derived
from the KIM model (Hong et al., 2018). The KIM model provided
simulated meteorological fields at a horizontal resolution of 0.125◦ ×
0.125◦ latitude-longitude with a temporal resolution of 3-h, which were
used as input for the STILT model. Five hundred particles were released
from an inlet height of 10 m above the ground across the YES-AQ vessel
route within a latitude range of 31.2–37.8◦ N and a longitude range of
124–125◦ E and traced backward in time for 2 or 5 days to generate air
mass footprints with a horizontal resolution of 0.27◦ × 0.27◦ and a time
resolution of 1-h. The single-particle backward trajectories were
computed at 3-h intervals using the HYSPLIT model. The back-trajectory
calculation required a three-dimensional velocity field obtained from
the Air Resources Laboratory, using the global data assimilation dataset
of the National Centers for Environmental Prediction (NCEP). These
footprints were used to identify the source-receptor relationship of
near-surface measurements of GHGs and reactive gases conducted by
the YES-AQ vessel campaign in March–April 2021. The footprint sensi­
tivity generated by the model simulation represents the potential source
distributions or footprints, reflecting the relative contribution from
different grid points.
4. Results and discussion
4.1. Latitudinal distribution of GHGs and air pollutants in the Yellow Sea
The research vessel completes two return journeys per day,
traversing the Yellow Sea at different times of the day, which can
sometimes complicate the analysis of data from such mobile platforms.
The prevailing winds in spring over the Yellow Sea are typically westerly
or easterly, resulting in measurements frequently sampling the outflow
from the Asian continent. Fig. 2 shows the latitudinal distributions of
CO2, CH4, CO, O3, NOx, and SO2 without accounting for temporal var­
iations. Additionally, we compared these latitudinal concentrations with
in-situ surface observations obtained from the AMY and GSN stations,
which are two WMO/GAW regional background stations in Korea
(Fig. 1).
The mean dry mole fractions of CO2, with an average of 425.5 ± 2.5
ppm, observed in the southern region below approximately 34.5◦ N
latitude, are comparable to the April monthly average level observed at
the GSN station (427.2 ± 3.4 ppm). However, a higher frequency of high
Fig. 3. The representative back-trajectory (centroid) and total frequency of occurrence of the clusters arriving at (a) 37.25◦ N, 124.32◦ E and (b) 35.5◦ N, 124.32◦ E (c)
33.25◦ N, 124.32◦ E at a height of 500 m.
5
Atmospheric Environment 317 (2024) 120201
levels was observed at northern latitudes above 35◦ N. Similarly, the
mean value of CO2, with 429.5 ± 2.5 ppm observed between 34.5 and
37.8◦ N, was comparable to that observed at the AMY station (433.3 ±
7.8 ppm). Similar patterns were observed for CH4, CO, SO2, and NOx,
with average values below 34.5◦ N comparable to those at the GSN sta­
tion, while concentrations sampled between 34.5 and 37.8◦ N were
comparable to those at the AMY station. This demonstrates that the
anthropogenic air pollutants observed in the Yellow Sea exhibit different
effects on air mass flow depending on latitude and that the GSN and
AMY stations, located in the southern and northern parts of Korea,
respectively, correspond well to the synoptic airflow transfer in the
Yellow Sea, especially during spring. The air mass transport flow can be
categorized based on the latitude range in the Yellow Sea during the
spring campaign period. Fig. 3 illustrates the centroid back-trajectory
(representative trajectory) with the total frequency of occurrence of
the cluster arrived at typical three passion (37.25◦ N 124.32◦ E; 35.5◦ N,
124.32◦ E; 33.5◦ N, 124.32◦ E) through the southern and northern regions
of Yellow Sea, during the research period. The cluster analysis of back-
trajectories shows more clear difference in air mass patterns in the
southern and northern regions of the Yellow Sea. Overall, the Yellow Sea
was predominantly influenced by fast Northwesterly wind in the spring
season, which is a prevailing wind pattern that brings well-mixed air
from high latitudes because of the development of Siberia high (Lee
et al., 2023). However, the air mass back-trajectories slowly passed
through Northern China, including the Bohai Sea, and Eastern China,
including the Shandong peninsula, before arriving at 37.25◦ N and
35.5◦ N latitude, respectively, both regions are close to highly industri­
alized areas in China (Li et al., 2020). In addition, before arriving at the
southern part of the Yellow Sea (33.25◦ N, 124.28◦ E), air mass slowly
passed through the Southern Ocean and the Korean peninsula, which is
one of the reasons for the observed differences in latitudinal gradients
over the Yellow Sea (high in the northern and low in the southern parts
of the Yellow Sea).
Notably, the latitudinal distributions of O3 and SO2 differed from
those of the other compounds. O3 was frequently sampled at higher
levels compared to the in-situ surface stations at AMY and GSN across
various latitudes. The average mean levels of O3 sampled in the Yellow
Sea were approximately 58.6 ± 20 ppb, which were higher than those
observed at the AMY background station (45.8 ± 11.5 ppb, monthly
mean with 1-σ standard deviations) during the same period and com­
parable to those from the GSN station (56.2 ± 10.2 ppb). This indicates
that the Yellow Sea was influenced by emissions of O3 from distant
source regions through long-range transport from March to April (Song
et al., 2009). Ozone pollution has become a severe environmental
S. Li et al.
problem, mainly in urban areas of China and Korea, owing to the
continued increase in O3 concentrations despite the decreasing level of
NOx, which is known as an O3 precursor (Kim et al., 2021; Wang et al.,
2021). The mean level of SO2 sampled in the Yellow Sea was about 1.3
± 0.3 ppb, slightly higher than that from the AMY station (0.9 ± 0.6
ppb) and GSN station (0.7 ± 0.6 ppb) within uncertainties. The lower
level of SO2 in the Yellow Sea and at both Korean GAW stations can be
attributed to a continuous decrease in the Asian region due to the cur­
rent desulfurization policy, especially in China (Wang et al., 2014, van
der A et al., 2017). The SO2 concentration has also decreased since 1987
owing to the abatement strategy to control air pollution emissions in
South Korea (Khan et al., 2017). Notably, highly elevated CH4 and O3
concentrations were simultaneously observed around 34.8◦ N. These
high plume events of CH4 and O3 will be analyzed in Section 4.4.
4.2. Potential source region determination by wind
In the Yellow Sea region, where direct pollution emissions are ab­
sent, highly elevated concentrations of various chemical compositions
are likely influenced by long-range transport. To investigate the impact
of different wind speeds and wind directions on these chemical com­
positions, we used a bivariate polar plot for stratified analysis, as shown
in Fig. 4. The polar plot illustrates that highly elevated mean concen­
trations appeared in different wind directions and wind speeds for each
compound. However, there are limitations in providing a more detailed
explanation of potential emission sources with wind directions using a
bivariate polar plot due to the mobility of the vessel being used as a
platform. Consequently, this study focuses solely on discussing westerly
or easterly wind directions, given the Yellow Sea’s location, to identify
evidence of regional emission sources, particularly originating from
either China or the Korean peninsula.
Mole fractions of CO2 (>440 ppm, higher than the observations of
433 ppm at the AMY station) were observed in easterly wind directions
under wind speeds of approximately >5 m/s. Similarly, a high plume of
CH4 (>2.05 ppm), which was elevated by approximately 0.1 ppm
compared to observations at the AMY station, also occurred with the
same wind patterns. However, another high plume of CH4 (>2.05 ppm)
was also detected in westerly wind directions under wind speeds of
approximately >7 m/s. This suggests that the elevated CH4 observed
over the Yellow Sea could be attributed to the potential emission source
areas in both the western and eastern parts of the Yellow Sea region.
Regarding CO, highly elevated mole fractions (>300 ppb) were observed
not only in the westerly wind direction under wind speeds greater than
5 m/s. CO was also elevated to a range of approximately 270–300 ppb
under wind speeds greater than 5 m/s under westerly wind direction.
Similarly, NOx showed similar patterns to CO, with high levels of NOx
(>13 ppb) detected in the westerly wind directions under wind speeds
ranging from 5 to 10 m/s. This suggests that the main hotspot regions for
CO > 300 ppb and NOx > 13 ppb were mostly located over the western
part of the Yellow Sea. Furthermore, O3 and SO2 also exhibited relatively
high concentration patterns in the westerly wind direction at high wind
speeds above 5 m/s. However, high levels of O3 (>100 ppb) were also
detected under a wind speed of approximately 7–8 m/s in the easterly
wind direction.
Overall, the main hotspot regions for highly elevated CO2 were
mainly attributed to the eastern region of the Yellow Sea. However,
emission source regions in the western part of the Yellow Sea also
contributed to highly elevated CO, NOx, and SO2. The main hotspot
regions for highly elevated O3 and CH4 appeared to be related to both
the eastern and western parts of the Yellow Sea. All these highly elevated
gaseous compounds were predominantly detected under high wind
speed conditions (≥5 m/s), suggesting that they were influenced by
long-range transported pollutants due to the absence of direct emission
sources in the Yellow Sea (Lee et al., 2023).
Additionally, CO2, CO, O3, and NOx concentrations were slightly
elevated under low wind speed conditions (<3 m/s), indicating that
6
Atmospheric Environment 317 (2024) 120201
some of the slightly elevated pollution could be attributed to small-scale
emission sources, such as fishing boats around research vessels. How­
ever, their influence appeared to be lower than that of pollution plumes
from the continent via long-range transport. To exclude the potential
effects of ship emissions in the vicinity of the research vessel, our
analysis in this study focused on wind speeds higher than 3 m/s.
Filtering out the effect of ship-borne emissions in close proximity to the
research vessel was beyond the scope of this work.
4.3. Identification of source characteristics based on correlation analysis
between CO2–CO–CH4
To investigate the source signatures of CO, CH4, and CO2, we
analyzed correlations between CH4 (ppm) versus CO (ppm) and CO
(ppm) versus CO2 (ppm) during the YES-AQ campaign (Fig. 5b). The
regression slope between CO2 and CO has been extensively used to
characterize regional source signatures (Halliday et al., 2019). Addi­
tionally, the correlation slope between CH4 and CO has been utilized to
identify emission sources by region, such as fossil fuel use, biomass
burning, and biogenic emissions (Baker et al., 2012). In this study, we
analyzed the relationship between CO, CH4, and CO2. As depicted in
Fig. S4, the majority of the observations exhibited a positive correlation
between CO and CH4. However, when the dry mole fraction of CH4 was
>2.05 ppm, the correlation with CO became less evident. Upon
removing the high CH4 (>2.05 ppm), the correlation coefficient
increased to R > 0.7, and the regression slope showed a value of 0.22
CH4 [ppm]/CO [ppm]. Notably, a previous study conducted at Hater­
uma Island, a remote station in Japan, during winter reported a
regression slope of 0.2–0.4, suggesting the influence of anthropogenic
emissions such as those from fossil fuel-related sources in East Asia
(Tohjima et al., 2014). If CH4 is impacted by strong anthropogenic
biogenic emission sources, the regression slope of CH4/CO would be
higher than 0.22 [CH4 (ppm)/CO (ppm)], as reported in previous studies
(Baker et al., 2012; Li et al., 2020).
The correlation slope between CO and CO2 has been extensively used
to characterize regional source signatures since the majority of atmo­
spheric CO comes from the incomplete combustion of carbon-containing
fuel (Ward et al., 1996). As shown in Fig. 5, the correlation between CO
and CO2 varied, indicating differences in combustion efficiency among
the sources. Considering the geographic location of the Yellow Sea be­
tween China and the Korean Peninsula, we employed an air mass
back-trajectory residence time analysis to categorize the data influenced
by each country. The classification method follows the approach out­
lined by Li et al. (2011) and is briefly described below. We calculated the
residence time of 5-day back-trajectories calculated using the HYSPLIT
model that arrived at the vessel’s route position with a spatial resolution
of 10 km using the method described in Poirot and Wishinski (1996). If
an air mass trajectory passed through mainland China or Korea under
the boundary layer height, the CO2 and CO data corresponding to the
residence time of the back trajectory within mainland China (or Korea)
were categorized. Approximately 86% of the total observations were
classified as being influenced by either China or Korea, indicating that
the Yellow Sea is suitable for monitoring air pollution from the Asian
continent. Two country domains were defined to separate
country-specific pollution signals from the original observations: the
Chinese domain, defined as the regional grid of 100–124◦ E and
21–45◦ N, and the Korean domain, defined as 126–128◦ E and 34–38◦ N.
As shown in Fig. 6, the majority of CO and CO2 observations that
passed through China have long data distributions that represent a “less
efficient” combustion sector, while those that passed through Korea are
situated in the “more efficient” combustion part. However, CO and CO2
exhibited consistent regression slopes regardless of whether they passed
through when CO was lower than approximately 300 ppb. The pollution
associated with “less efficient combustion” appears to be caused by CO
plume events with concentrations >300 ppb, which primarily originate
from China. The elevated levels of CO and CO2, indicative of their origin
S. Li et al. Atmospheric Environment 317 (2024) 120201

Fig. 4. Bivariate polar plot of (a) CO2, (b) CH4, (c) CO, (d) O3, (e) NOx, and (f) SO2 based on 1-min average data obtained during the YES-AQ campaign in
March–April 2021. The color scale indicates the mole fractions for each compound, and the radial scale shows the wind speed (m/s), which increases radially
outward from the center of the plot.

7
S. Li et al.
Fig. 5. (a) Scatter plot depicting the relationship between CO and CO2 with CH4, as well as between CH4 and CO with CO2, after removing data from the high CH4
plume (>2.05 ppm) observed during the 2021 YES-AQ campaign period from March to April.
Fig. 6. Regression slope analysis between CO and CO2 classified by origin. Red
dots represent air masses from China, while black dots represent the air masses
affected by Korea. These two groups can explain approximately 83% of the
observed data during the 2021 YES-AQ campaign.
in China, depend on whether the air mass passed through emissions
source regions and the speed at which it reached the receptor station. To
investigate the potential source distributions of high CO plumes, we
analyzed the air mass residence time using a statistical back-trajectories
method when CO levels exceeded about 350 ppb. The high plume of CO
appears to be associated with emissions potentially originating from
Northeastern China, including the Liaoning, Hebei, and Jiangsu Prov­
ince, where industrial regions are located (Fig. S5) (Kim et al., 2023).
The regression slope between CO (ppm) and CO2 (ppm) that originates
from China (Korea) is estimated to be 1.7% (0.5%) (denoted as CO
(ppm)/CO2 (ppm) × 100), which is comparable to that reported in
previous studies (Halliday et al., 2019; Li et al., 2020), where the
regression slope between CO and CO2 was above 1.8–2%. Combustion
efficiency has been improving in China owing to enhanced emission
control technology and government pollution control actions (Wei et al.,
2020; Zheng et al., 2018b). Therefore, continuous monitoring of the
CO/CO2 regression slope in regions such as the Yellow Sea area, which
effectively monitors long-range transported pollutants from Asian con­
tinents, is necessary (Li et al., 2020).
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Atmospheric Environment 317 (2024) 120201
4.4. Source identification of high plume of CH4, O3, SO2, and NOx
In this section, we examine the high plume observations of CH4, O3,
SO2, and NOx during the YES-AQ campaign. As shown in Fig. 7, a
noteworthy observation is that the maximum CH4 plume of approxi­
mately 2.1 ppm was recorded on April 22nd, coinciding with the
maximum O3 concentrations. As discussed in Section 3.2, CH4 dry mole
fractions exceeding 2.05 ppm did not exhibit a significant positive cor­
relation with either CO2 or CO, suggesting that the high plume may not
have originated from fossil fuel-related emission sources. To identify the
potential main source region for high plumes of CH4, air mass sensitivity
and XCH4 retrieval from TROPOMI/S5P were analyzed on April 22,
2021. Back-trajectories of air masses arriving at seven-point coordinates
(covering a latitude range of 35.4–36.6◦ N), where the vessel passed
between 7 a.m. and 9 PM in Korean time, were calculated using the
STILT model coupled with the KIM simulated 12 × 12 km meteorolog­
ical data, as detailed in Kenea et al. (2023b). From the backward air
mass sensitivity test, we found that the southwest part of the region is
primarily attributed to high CH4 concentrations (Fig. 8a), which is
consistent with the XCH4 hotspot regions detected from TROPOMI/S5P
satellite data (Fig. 8b). A previous report has shown that the south­
western region of Korea exhibited a surprisingly high CH4 plume from
aircraft measurements in the summer, potentially attributed to biogenic
emissions, such as landfill, livestock, and rice paddy agricultural activ­
ities in Korea (Li et al., 2020).
According to the National GHG inventory (GIR, 2022), most methane
emissions in South Korea originate from the agriculture sector (>40%),
and approximately 54% of Korea’s total agricultural land is used for rice
paddies (Korean Statistical Information Service, 2019). Furthermore, all
Fig. 7. Time series of CH4 (red) and O3 (gray) of 1-min interval data observed
on April 22nd, 2021 during the YES-AQ campaign.
S. Li et al. Atmospheric Environment 317 (2024) 120201

Fig. 8. (a) 5-day backward trajectory footprint using the Korean Integrated Model (KIM)-Stochastic Time-Inverted Lagrangian Transport (STILT) arriving over the
Yellow Sea between the 34–36◦ N, 124◦ E points on April 22nd. (b) The column-averaged dry mole fraction of CH4 retrieved from TROPOMI//S5P satellite data for
April 2021 along all satellite tracks passing through the Korean domain.

the top 15 administrative cities with high CH4 emissions from rice
paddies are situated in western Korea (Choi et al., 2018). Notably, the
relative soil moisture (at a soil depth of 5 cm; Fig. 9a) in the southwest
part of the region was more pronounced compared to other areas, and
the soil temperature (at a depth of 5 cm; Fig. 9b) was recorded to be
above approximately 16 ◦ C on April 21st to 22nd over the southwestern
region of Korea. Additionally, Kenea et al. (2021) demonstrated that
sudden increases in CH4 dry mole fractions observed at the AMY station
in Korea are related to biogenic emissions, which increase owing to
rising temperature and soil humidity. Hence, it is also possible that the
high-level CH4 observed during the YES-AQ campaign, which did not
exhibit a clear correlation with CO, was long-range transported from
biogenic emission sources such as agriculture from the southwestern
part of Korea, rather than from fossil fuel emissions. To better under­
stand this emission hotspot during the spring season, originating from
biogenic emissions sources, further investigations are required. Future
studies may benefit from additional data, such as stable carbon isotope
analysis of CH4, to characterize and define the emissions more
accurately.
As discussed in the preceding chapter, O3 concentrations remained
consistently high over the latitudinal sector in the Yellow Sea, frequently
exceeding those recorded at the AMY in-situ station. The highest O3
concentration during the 2021 YES-AQ campaign was 110.3 ppb,
recorded on April 22nd. On that day, O3 concentrations exceeding 80
ppb were continuously observed throughout the north-south route
during a period when wind speeds exceeded 3 m/s (Fig. 7). The highest
surface O3 concentration recorded by the AMY station during the same
period was 61 ppb. Considering that the monthly background concen­
tration at the AMY station in April 2021 was about 47.8 ppb (KMA,
2021), the O3 concentration observed on April 22nd was two to three
times higher. During the 2021 YES-AQ campaign, the observed surface
O3 concentrations over the southwestern part of Korea showed a range
of 49–98 ppb from the 21st of April (Fig. S6). Notably, this concentration
range was slightly lower than the O3 levels observed over the Yellow
Sea, which ranged from 80 to 110 ppb during the same period. The
vessel route was located approximately 200 km away from the potential
source region in southwestern Korea. Given this distance and the
recorded highest atmospheric temperature of 18 ◦ C on 22nd April during
the campaign period, the elevated ozone levels may also be attributed to
formation during transport in the polluted plumes (Lal et al., 2006).
Previous studies have shown that high concentrations of O3 in urban
areas of the Korean Peninsula are often caused by continental tropical

Fig. 9. (a) The relative soil moisture (%) and (b) soil temperature (◦ C) at 5 cm soil depth over South Korea on April 21st. The observation data were provided by
Automated Agricultural Observing System (AAOS) networks in the Korean Meteorological Administration and are available at https://data.kma.go.kr/data/.

9
S. Li et al.
air masses, where the surface temperature rises and the relative hu­
midity decreases (Kim et al., 2021).
The high plume of NOx, as depicted in Fig. 2e, was consistently
observed above the AMY measurements for a continuous period of two
days between March 29th and 30th, with an average concentration of
approximately 15 ppb. This time period coincided with an extremely high
Asian dust event, as evidenced by the vessel’s detection of elevated PM10
levels from March 28th to 30th and the KMA issuing an Asian dust
warning, the first in five years, due to PM10 mass concentrations exceeding
800 μg/m3. Maximum levels of SO2 (about 4 ppb) were also detected on
March 30th, albeit for a brief duration of 1–2 h when the vessel passed
through the southern part between 35.4 and 36◦ N. Significant positive
correlations were observed between NOx and SO2, with an SO2/NOx ratio
of 0.16, as shown in Fig. 10. A high SO2/NOx ratio (>0.6) indicates sig­
nificant contributions from industrial point sources, whereas a low ratio
(0.04–0.12) signifies more contributions from mobile sources (Aneja et al.,
2001; Halim et al., 2018). A previous study reported a high long-term
SO2/NOx ratio (>0.6) in Jiangsu Province in Eastern China, attributed to
a dominant industrial source (Wang et al., 2021). This suggests that the
low occurrence frequency of SO2 concentrations exceeding 1.5 ppb in the
Yellow Sea on March 30th is unlikely to be attributed to industrial point
sources from Eastern China but rather to mobile sources. SO2 concentra­
tions over the Yellow Sea were generally low, with almost 80% of the
sampled data <1.5 ppb, and the maximum level not exceeding 4 ppb
during the YES-AQ campaign. Therefore, it is challenging to identify the
main hotspot regions of SO2. In this part of the study, we focus more on the
highly elevated NOx levels observed over the two-day period.
To track the origin of the maximum concentrations of NOx observed
on March 29–30th, a footprint analysis using KIM-STILT with only 2-day
backward trajectories was performed. The analysis revealed that the
majority of the air mass passed through the Bohai Sea region before
reaching the Yellow Sea (see Fig. 11a). This finding is consistent with the
NO2 retrieval from the TROPOMI/S5P satellite on March 29–30th
indicating the high NO2 retrieval over the Bohai Sea, which appears to
be transported from the surrounding region and enclosed in this region
(see Fig. 11b). Bohai Sea is surrounded by highly industrialized areas
and is semi-enclosed, and its pollution status has aroused many con­
cerns. The pollutants transported and enclosed in the Bohai Sea seem to
be mainly affected by emissions from Eastern and Northern China due to
the storage of westerly wind patterns (see Fig. S7).
Fig. 10. Scatter plot between SO2 and NOx with latitude observed on March
29–30. The longitude did not change significantly during the two days. The
fitted line of regression analysis (black) shows the relationship between SO2 and
NOx with data observed between 35.4 and 36◦ N latitude.
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Atmospheric Environment 317 (2024) 120201
5. Conclusions
In this study, we analyzed the spatial distribution and correlation
among greenhouse gases (CO2 and CH4) and reactive gases (CO, NOx,
SO2, and O3) collected via a research vessel during the YES-AQ
campaign period in March–April 2021. The main findings of this study
are summarized as follows.
(1) We observed a clear latitude gradient of the anthropogenic
composition (e.g., CO2, CH4, CO, NOx) in the Yellow Sea with
good correspondence between observations from two WMO/
GAW stations located in the southern part (GSN) and the northern
part (AMY) within the latitude range of 31.2–37.8◦ N
(2) However, O3 concentrations were consistently higher across
different latitudes in the Yellow Sea compared to the in-situ
surface stations at AMY and GSN, suggesting the influence of
long-range transport from areas with strong O3 emissions or
photochemical formations during transport in the polluted plume
over the Yellow Sea.
(3) We observed a significant positive correlation between CO and
CH4 with a slope of 0.2[CH4 (ppm)/CO (ppm)], after excluding
high CH4 concentrations (>2.05 ppm), indicating a potential
fossil fuel-related source. Furthermore, we observed different
regression slopes for CO and CO2 depending on regional char­
acteristics, particularly in air originating from Korea (0.5% [CO
(ppm)/CO2 (ppm) x 100]) and China (1.7%).
(4) A considerably high plume of CH4 (>2.05 ppm) was predomi­
nantly observed on April 22, 2021, in the Yellow Sea, likely due
to biogenic emissions in the southwestern region of Korea. This is
based on the KIM-STILT footprint analysis, XCH4 retrieval from
the TROPOMI/S5P satellite, and soil moisture/temperature
analysis in the potential source region.
(5) High plumes of NOx and SO2 were detected during the period of
March 29–30, 2021, which coincided with an extremely high
Asian dust event with PM10 mass concentrations of >800 μg/m3.
KIM-STILT analysis revealed that the majority of the high plume
of NOx is attributed to Northern China and Bohai Bay.
This study has identified the sources and drivers of the enhancements
by examining co-variations in CO2, CH4, CO, O3, NOx, and SO2 through
high-resolution vessel observation in the Yellow Sea during the YES-AQ
campaign. The findings demonstrate the critical role of vessel observa­
tions in understanding the spatial and temporal variations, identifying
emissions sources, and addressing transboundary air pollution issues.
The processes driving the changes in GHGs and air pollutants in East
Asia have a significant impact on the global carbon cycle and human
health. Given its strategic geographical position, the Yellow Sea pro­
vides an effective monitoring of the carbon cycle, climate change, and
emissions of both China and Korea.
Funding
This research was funded by the Korea Meteorological Administra­
tion’s Research and Development Program “Developing Technology for
Integrated Climate Change Monitoring and Analysis” under grant
(KMA2018-00324).
CRediT authorship contribution statement
Shanlan Li: Sample collection and, Formal analysis, Data integra­
tion, Result analysis, Formal analysis, Data curation, Investigation,
Writing – original draft. Samuel Takele Kenea: Methodology, Valida­
tion, Writing – review & editing. Sumin Kim: Investigation, Sample
collection and, analysis. Hee-Jung Yoo: Investigation, Sample collec­
tion and, Formal analysis. Sangwon Joo: Validation, Writing – review &
editing. Haeyoung Lee: Sample collection and, Formal analysis, Writing
S. Li et al.
Fig. 11. (a) Column-averaged dry mole fraction of NO2 retrieved from TROPOMI/S5P satellite data for March 30th, 2021, along all satellite tracks passing through
the East Asian domain. (b) Two-day backward trajectory footprint using KIM-STILT model arriving over the Yellow Sea between 34 and 36◦ N, 124◦ E points on
March 30th.
– review & editing. Sangmin Oh: Sample collection, Writing – review &
editing. Min Jae Jeong: Sample collection, Writing – review & editing.
Wonick Seo: Formal analysis, Writing – review & editing. Miyoung Ko:
Sample collection, Writing – review & editing. Soojeong Lee: Sample
collection, Writing – review & editing. Young-Suk Oh: Writing – review
& editing. Daegeun Shin: Writing – review & editing.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgments
The authors would like to thank the payload operation team, tech­
nicians, and KMA’s research vessel management team for their signifi­
cant contributions to the YES-AQ campaign. We are also grateful to the
NOAA science team for providing us with meteorological reanalysis
data, and NOAA’s Air Resources Laboratory for providing the HYSPLIT
transport and READY website (http://www.ready.noaa.gov). Addition­
ally, we acknowledge the TROPOMI/S5P Science teams for providing
NO2 and CH4 data.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.atmosenv.2023.120201.
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