journal of environmental sciences 135 (2024) 656–668

Available online at www.sciencedirect.com

www.elsevier.com/locate/jes

MAX-DOAS and in-situ measurements of aerosols

and trace gases over Dongying, China: Insight into
ozone formation sensitivity based on secondary
HCHO

Xiaojun Zheng 1,∗∗, Zeeshan Javed 1,∗∗, Cheng Liu 2,3,4,5,∗, Aimon Tanvir 6,
Osama Sandhu 7, Haoran Liu 8, Xiangguang Ji 8,9, Chengzhi Xing 3,
Hua Lin 10, Daolin Du 1,∗
1 Institute of Environment and Ecology, School of the Environment and Safety Engineering, Jiangsu University,
Zhenjiang 212013, China
2 Department of Precision Machinery and Precision Instrumentation, University of Science and Technology of China,

Hefei 230026, China

3 Key Laboratory of Environmental Optics & Technology, Anhui Institute of Optics and Fine Mechanics, Hefei

Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China

4 Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of

Sciences, Xiamen 361021, China

5 Key Laboratory of Precision Scientific Instrumentation of Anhui Higher Education Institutes, University of Science

and Technology of China, Hefei 230026, China

6 Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental

Science and Engineering, Fudan University, Shanghai 200433, China

7 National Agromet Center, Pakistan Meteorological Department, Islamabad 44000, Pakistan
8 Institute of Physical Science and Information Technology, Anhui University, Hefei, 230601, China
9 Information Materials and Intelligent Sensing Laboratory of Anhui Province, Anhui University, Hefei, Anhui

230601, China
10 School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China,

Hefei, 230026, China

a r t i c l e i n f o a b s t r a c t

Article history: This study presents a comprehensive overview of the atmospheric pollutants including Sul-
Received 12 April 2022 fur dioxide (SO2 ), Nitrogen dioxide (NO2 ), Formaldehyde (HCHO), Particulate Matter PM; PM10 :
Revised 31 August 2022 diameter ≤ 10 μm, and PM2.5 : diameter ≤ 2.5 μm), and Ozone (O3 ), over Dongying (Shandong
Accepted 12 September 2022 Province) from March-April 2018 and September-October 2019 by employing ground-based
Available online 24 September 2022 Multiple Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations along
with the in-situ measurements attained by the national air quality monitoring platform. The
concentrations of SO2 and NO2 were under the acceptable level, while both PM2.5 , and PM10

∗
Corresponding authors.
E-mails: Chliu81@ustc.edu.cn (C. Liu), ddl@ujs.edu.cn (D. Du).
∗∗
These authors contributed equally to this work.

https://doi.org/10.1016/j.jes.2022.09.014
1001-0742/© 2023 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
 journal of environmental sciences 135 (2024) 656–668 657

Keywords: were higher than the safe levels as prescribed by national and international air quality stan-
MAX-DOAS dards. The results depict that 21% of the total observation days were found to be complex
Trace gases polluted days (PM2.5 > 35 μg/m3 and O3 > 160 μg/m3 ). The secondary HCHO was used for ac-
Ozone sensitivity curate analysis of O3 sensitivity. A difference of 11.40% and 10% during March-April 2018 and
Secondary HCHO September-October 2019 respectively in O3 sensitivity was found between HCHOtotal /NO2
Complex Pollution and HCHOsec /NO2 . The results indicate that primary HCHO have significant contribution in
HCHO. O3 formation predominantly remained to be in VOC-limited and transitional regime
during March-April 2018 and September-October 2019 in Dongying. These results imply that
concurrent control of both NOx and VOCs would benefit in ozone reductions. Additionally,
the criteria pollutants (PM, SO2 , and NO2 ) depicted strong correlations with each other ex-
cept for O3 for which weak correlation coefficient was obtained with all the species. This
study will prove to be baseline for designing of air pollution control strategies.
© 2023 The Research Center for Eco-Environmental Sciences, Chinese Academy of
Sciences. Published by Elsevier B.V.

PM2.5 , diameter ≤ 2.5 μm) and carbon monoxide (CO). These

Introduction six pollutants are considered as key while developing policies
and designing pollution control strategies. Several control reg-
Atmospheric pollution has gained much attention during the
ulations were adopted at national, provincial and metropoli-
past decade owing to acute impacts on ecosystem and human
tan levels to combat these pollutants. These measures which
health. Rapid urbanization, industrialization and increasing
include optimization of industrial structure, reduction of coal
use of fossil fuels to meet the demands of booming population
usage, increase in share of clean energy sources and instal-
are deemed as the important aspects that lead to deterioration
lation of installation of fuel gas desulfurization (FGD) devices
in air quality, consequently posing serious threat to human
have been significantly effective in controlling the criteria pol-
health (Tian et al., 2018; Cheng et al., 2019a; Li et al., 2020a;
lutants including NO2 , SO2 , and PM10 (Wang et al., 2021). How-
Yin et al., 2021; Zhou et al., 2021). Air pollution in China during
ever, it is worth to mention that these strategies are not effec-
the 21st century accords with the fast-paced urban develop-
tive enough to control near-ground PM2.5 and the secondary
ment and rapid economic growth (Zhou et al., 2021). Owing to
pollution problem marked by excessive O3 due to their com-
significant population and clustered industrial sectors, which
plex pollution sources (Dai et al., 2021; Li et al., 2019a; Qin et al.,
enhance fossil fuel combustion by vehicular transport and in-
2021). Therefore, this needs to be studied further by analysing
dustrial activities, urban areas are more prone to experience
O3 sensitivity to its precursors, to come up with efficient policy
high pollution levels and deteriorated air quality (Tian et al.,
towards controlling O3 pollution in China. The other main pol-
2018).
lution issue currently in China is a phenomenon in which high
In wake of the severity of the atmospheric pollution prob-
O3 and high PM2.5 coincided beyond the National Ambient Air
lem, China had started air quality monitoring network in 2013
Quality Standards (NAAQS) (Dai et al., 2021; Qin et al., 2021).
with monitoring stations all across the country. The measure-
This condition is termed as a complex pollution in this study
ments taken at these monitoring stations have been used to
here-after, where the daily mean PM2.5 concentration exceeds
analyze the characteristics of different air pollution episodes
35 μg/m3 , and the daily mean O3 concentration exceeds 160
in various regions of China (Qin et al., 2021; Sulaymon et al.,
μg/m3 on the same day.
2021; Rupakheti et al., 2021; Li et al., 2020a). For the past
The oxides of nitrogen (NOx) and volatile organic com-
few decades, the use of remote sensing techniques to mon-
pounds (VOCs) are the major precursors for O3 formation. NO2
itor air quality has also got huge attention. Remote sensing
constitutes a major portion of NOx and is, therefore, used for
techniques include both ground and satellite-based instru-
O3 sensitivity studies. It is a crucial atmospheric pollutant
ments to carry out three dimensional (3-D) observations of
coming from anthropogenic sources mainly fossil fuel com-
the atmosphere. The Multi Axis Differential Optical Absorp-
bustion (Vinken et al., 2014) and plays a key role in tropo-
tion Spectroscopy (MAX-DOAS) is one of the remote sensing
spheric O3 formation as well as the generation of hydroxyl
techniques that is used to monitor trace gases and aerosol
(OH) radicals (Cheng et al., 2019b). The OH radicals play an
pollutants in the atmosphere by employing Beer-Lambert law
important role in the atmospheric chemical processes espe-
(Wagner et al., 2011; Platt and Stutz, 2008; Hönninger et al.,
cially contributing the formation of secondary aerosols and
2004; Bobrowski et al., 2003). Owing to relatively low opera-
nitric acid (Huang et al., 2014; Zhao et al., 2018), making it a
tional cost and easy installation, the MAX-DOAS instrument is
critical reduction target for the policymakers. Formaldehyde
widely being used to monitor atmospheric species for ground-
(HCHO) is the most abundant aldehyde in the atmosphere
based, satellite based, ship-based, vehicle-mounted and air-
which comes as an oxidation product of VOCs in the atmo-
borne observation platforms (Zhou et al., 2021).
sphere, thereby serving as an ideal proxy for VOCs (Javed et al.,
The Ministry of the Environmental Protection of the Peo-
2019a; Tanvir et al., 2021). Upon photolysis, this gas gener-
ple’s Republic of China classified nitrogen dioxide (NO2 ) and
ates HO2 free radicals which then react with NO to generate
sulfur dioxide (SO2 ) as criteria pollutants along with ozone
OH radicals, thereby playing an important role in defining at-
(O3 ), particulate matter (PM: PM10 , diameter ≤ 10 μm; and
mospheric chemistry (Tian et al., 2018). The ratio of HCHO to
658 journal of environmental sciences 135 (2024) 656–668
NO2 (RFN) is a common method employed to study the sen-
sitivity of O3 to its precursor species. Nonetheless, in case of
higher primary emissions of HCHO (>50%), the corresponding
ratio of HCHO/NO2 is likely to be overestimated, thereby mis-
diagnosing numerous VOC-limited scenarios as NOx-limited
(Xue et al., 2022). Hence, the accurate analysis of O3 -NOx-
VOC sensitivity can more arguably be possible with secondary
HCHO. Considering the aforementioned scenario of O3 pollu-
tion in China, the study of O3 sensitivity based on secondary
HCHO is crucial, in different regions of China with discrete cli-
matic characteristics.
The atmospheric quality in China has been extensively
studied using the MAX-DOAS instrument over various cities
of China located in different regions including Beijing-Tianjin-
Hebei region (Jing–Jin–Ji (JJJ) in Chinese) (Zhang et al., 2016),
Pearl River Delta (PRD) region (Ding et al., 2017), and Yangtze
Rivere Delta (YRD) region (Javed et al., 2021). Despite being
economically crucial, there exist sparse studies on air pollu-
tion in Shandong Province. Using the data from the Depart-
ment of Ecological Environment of Shandong Province from
2013 to 2019, Zhao et al. (2021) reported trends in the con-
centrations of air pollutants along with the impact of meteo-
rology. Zhong et al. (2022) studied the inter-annual variations
of six criteria pollutants over Shandong province by employ-
ing data from the National Air Quality Monitoring Network
(NAQMN) from 2014 to 2018. Xing et al. (2022) reported the air
quality over Shandong province before and after the COVID-
19 using satellite observations. Some studies have been re-
ported over different cities of Shandong Province including
Jinan (Cui et al., 2020; Zhang et al., 2017a), Weifang (Li et al.,
2019b), and Qingdao (Li et al., 2017). However, there is no re-
ported study on O3 sensitivity to its precursors and status of
complex air pollution episodes in Shandong.
The current study uses MAX-DOAS observations and in-
situ measurements of trace gases and particulate matter dur-
ing March-April 2018 and September-October 2019 in Dongy-
ing, Shandong. The two different time periods i.e. March-
April 2018 and September-October 2019 were used to examine
the variation in trace gases, particulate matter and pollution
episodes during different seasons. The economy of the city
thrives on crucial oil exploration activities which is why air
quality monitoring of the city is highly important. The main
objective of this study is to report current status of air pollu-
tion and occurrence of complex pollution episodes and iden-
tification of ozone sensitivity based on secondary HCHO. This
study is unique and vital due to different prospects to the best
of author’s knowledge 1) it is first study to report O3 sensitivity
to its precursors in Shandong province 2) secondary HCHO is
utilized to identify ozone sensitivity instead of primary HCHO
3) it is first study to report complex air pollution episodes in
Dongying city.
1. Methodology
1.1. Description of the study area
Dongying city lies on the northern side of Shandong province
in China (Fig. S1). The area has a terrain which inclines in
the direction of the Yellow River from the southwest to the
northeast. The climate is characterized by hot and rainy sum-
mer, shorter and humid spring, and a dry and cold winter.
The MAX-DOAS instrument was mounted at (36°55 –38°10 N,
118°07 –119°10 E) in Dongying. The site selected for the exper-
iment was located near the Yellow River estuary at the Yel-
low River Delta Coastal Wetland Ecological experiment sta-
tion. This site is around 50 km away from urban Dongying near
S228 provincial highway with reed as the dominant vegeta-
tion.
1.2. MAX-DOAS instrument
The observations of several trace gases are carried out us-
ing the MAX-DOAS (Multi-AXis DOAS) instrument which is
based on Differential Optical Absorption Spectroscopy (DOAS)
technique which mainly consists of a spectrometer (Avaspec-
UL2048L-USB2) with spectral range between 300–460 nm and
resolution of 0.6 nm. Scattered sunlight is used as principal
source of light by the instrument while the spectral observa-
tions to retrieve information about the species of concern are
made at various viewing angles (Plane and Saiz-Lopez, 2007).
A built-in processor mechanically controls the everyday mea-
surements made by the MAX-DOAS.
1.3. DOAS analysis
Accurate tropospheric columns of trace gas species are re-
trieved using the MAX-DOAS instruments which are capable
of performing measurements at various elevation viewing an-
gles called as EVAs (1°, 2°, 3°, 4°, 5°, 6°, 8°, 10°, 15°, 30°, and
90°). The technique reduces the contributions of the strato-
sphere to the tropospheric measurements by employing the
zenith angle as reference. The obtained spectra were analysed
via QDOAS software (version 2.109.4) established by BIRA-IASB
(Danckaert et al., 2013; Javed et al., 2019b). In order to come up
with the finest possible retrieval settings for the concerned
species, several sensitivity tests were performed. Table 1 de-
scribes the retrieval settings used for the current analysis
incorporating the best suited wavelength window and the
absorption cross-sections for fitting algorithm. Furthermore,
high-resolution solar spectrum was utilized to calibrate wave-
length (Chance and Kurucz, 2010). The spectra were adjusted
for offset and dark current before performing the spectral
analysis.
For each scanning series, the spectral fitting at various
viewing angles was ensured by selecting Fraunhofer reference
at 90°. Thus, differential slant column densities (dSCDs) are
obtained as an outcome. Owing to the scattering processes in
the atmosphere, the quality of data is likely to be impacted. In
order to minimize the contribution of atmospheric scattering
processes and improve the data quality, the measurements at
solar zenith angle (SZA) higher than 75° and root mean square
(RMS) more than 0.004 were filtered out. The spectral DOAS fit
for HCHO, SO2 and NO2 at elevation angle 2° is shown in Fig.
S2. Differential air mass factors (DAMFs) were utilized for the
calculation of tropospheric vertical column density (VCDtrop )
(Wagner et al., 2010; Solomon et al., 1987).
 journal of environmental sciences 135 (2024) 656–668 659

Table 1 – Retrieval settings for the analysis of SO2 , NO2 , and HCHO.

Cross-sections Data source Trace gases

SO2 NO2 HCHO

√ √
HCHO 297 K, (Meller and Moortgat, 2000) X
√ √ √
NO2 220 K, (Vandaele et al., 1998)
√ √
SO2 298 K, (Vandaele et al., 1998) X
√ √ √
O3 243 K, (Fleischmann et al., 2004)
√ √ √
O3 223 K, (Serdyuchenko et al., 2014)
√ √
O4 293 K, (Thalman and Volkamer, 2013) X
√ √ √
BrO 223 K, (Fleischmann et al., 2004)
√ √ √
Ring Calculated with QDOAS
Polynomial degree 5 5 5

The vertical column densities (VCDs) are calculated from regression model, given by Eq. (8).
the dSCDs of trace gases using dAMFs (Liu et al., 2016).
[HCHO] = α0 + α1 [CO] + α2 [Ox ] (8)
dSCDα
VCDtrop = (1)
dAMFα where, α 0 , α 1 , and α 2 denote fitting coefficients of the model, α 0
represents the background HCHO. The background levels can-
where, α denotes the elevation angle used for making the cor-
not be enumerated into either primary or secondary sources
responding observation, dAMF is calculated as:
of emission. The [HCHO] shows level of HCHO, [CO] represents
concentration of CO, and [Ox ] depicts Ox concentration. The
dAMF = AMFα − AMF90◦ (2)
relative contribution of primary, secondary, and background
HCHO to the ambient HCHO can be computed by employing
dSCDα the following equations.
VCDtrop = (3)
AMFα − AMF90◦
Geometric approximation is used to calculate AMF HCHO primary = α1 (CO )/HCHO × 100% (9)
(Tan et al., 2018):

1 HCHOSecondary = α2 (Ox )/HCHO × 100% (10)

AMF = (4)
Sin (α)

Eq. (3) now implies: HCHObackground = α0 /HCHO × 100% (11)

where, HCHOprimary , HCHOSecondary and HCHObackground signify

dSCDα
VCDtrop = (5) the contributions of primary, secondary, and background
1
Sin(α)
−1 HCHO, respectively.
A simplified equation was employed to convert HCHO
1.4. Error estimation DSCDs to ground surface mixing ratios of HCHO (ppbv). Ma-
jority of the previously published literature over China reports
For the MAX-DOAS observations, the error is estimated by con- that HCHO in the atmosphere is mostly concentrated in the
sidering DOAS fitting error. lower atmosphere (i.e., below 1km) (Chan et al., 2019). Hence,
Eq. (6) represents the fitting error of the DOAS to the ob- the mixing ratios are calculated here by using the following
served VCDs: Eq. (12).

VCDerror 1.25 × DSCD mol/cm2 )
VCD f itt ing error = (6) Rppbv = (12)
VCD a × P
here, R denotes mixing ratio for HCHO, a is termed as the
√    
2 dSDs2α=90◦ + dSDs2α=90◦ unit conversion factor of DU to mol /cm2 and is equal to
=   (7)
2.688 × 1016 , DSCD represents HCHO VCDs, while p denotes
2 Sin1(α) − 1 × VCD
the difference in pressure between the surface and at 1 km
For our study, the hourly error means around 15% for (Ziemke et al., 2001).
HCHO, 12% for NO2 and 17% for SO2 .
1.6. Ancillary data
1.5. Linear regression model
In situ measurements for the criteria pollutants including
By employing CO and Ox (NO2 + O3 ) as tracers, primary NO2 , SO2 , CO, O3 , PM10 and PM2.5 were attained from national
and secondary ground-surface sources HCHO can be distin- online database for air quality analysis and monitoring plat-
guished. The sources of HCHO can be enumerated by linear form (http://www.cnemc.cn/). The data is available online and
660 journal of environmental sciences 135 (2024) 656–668
Fig. 1 – Time series of MAX-DOAS observed VCDs for (a) SO2 , (b) HCHO, and (c) NO2 at elevation angle 2° at Dongying during
March-April 2018 and September- October 2019.
the monitoring stations are managed by China National En-
vironmental Monitoring Center. The daily mean concentra-
tion of these measurements spanning from 01st March- 30th
April 2018 and 1st September 2019-30th October 2019 was used
in this study. ERA5 reanalysis data for meteorological param-
eters (relative humidity, temperature, wind speed and wind
direction) over Dongying were obtained from the Copernicus
Data Hub (available online: https://cds.climate.copernicus.eu,
last accessed on 14 October 2021). The time series of temper-
ature, relative humidity, wind speed and wind direction over
Dongying for observation period are shown in Fig. S3. The tem-
perature, relative humidity and wind speed ranges from 1°C
- 24°C, 24%-90%, 1–7 m/sec respectively during March-April
2018. Whereas during September – October 2019 temperature,
relative humidity and wind speed ranges from 7°C-27°C, 37%-
97%, 2–17 m/sec.
2. Results and discussions
2.1. Timeseries for MAX-DOAS and In-situ observations
The time series of (a) SO2 , (b) HCHO, and (c) NO2 for the
study period over the studied site are shown in Fig. 1. As
evident from the figure, the study period has been split to
two distinct time periods for March-April 2018 and October-
November 2019. During 2018, the observation period lays in
the spring while for 2019, the observations were made during
autumn. The minimum, maximum and mean SO2 VCDs re-
mained to be 1.28×1016 mols/cm2 , 5.54 ×1016 mol/cm2 , and
2.89 ×1016 mol/cm2 respectively during March-April 2018,
while 1.67×1015 mol/cm2 , 4.32×1016 mol/cm2 , and 1.68×1016
mol/cm2 respectively for September-October 2019. For HCHO,
the minimum, maximum and mean VCDs was found to
be 2.28×1016 mol/cm2 , 4.61×1016 mol/cm2 , and 3.57×1016
mol/cm2 respectively during 2018, while 1.78×1016 mol/cm2 ,
7.85×1016 mols/cm2 , and 2.99×1016 mol/cm2 respectively dur-
ing 2019. The NO2 vertical columns over the observation site
depicted minimum, maximum and mean values of 2.42×1016
mol/cm2 , 6.95×1016 mols/cm2 , and 3.38×1016 mol/cm2 respec-
tively for 2018, and 1.75×1015 mol/cm2 , 8.48×1016 mol/cm2 ,
and 3.65×1016 mol/cm2 respectively for 2019. It is notewor-
thy that the mean concentrations of all the observed species
during 2018 and 2019 remained to be almost identical de-
spite the fact the observations were made in different sea-
sons. It has already been established in literature that the con-
centrations of these trace gas species remain almost iden-
tical during spring and autumn which can be attributed to
 journal of environmental sciences 135 (2024) 656–668
Fig. 2 – Time-series of In-situ Measurements in Dongying where dashed lines indicate NAAQS Grade 1 standard and dotted
lines indicate Grade 2 standard.
the identical sources of emissions during these two sea-
sons (Xue et al., 2022; Hong et al., 2022; Rupakheti et al.,
2021), for instance, biogenic emissions in case of HCHO
(Chan et al., 2019).
The in-situ measurements of particulate matter and trace
gases from the national environment monitoring station
taken at observation site are depicted by the time series in
Fig. 2. The mean concentrations of SO2 , NO2 , O3 , PM2.5 , PM10 ,
and CO in Dongying as a whole ranged from 6 to 39 μg/m3 , 8
to 73 μg/m3 , 61-232 μg/m3 , 12-149 μg/m3 , 36-223 μg/m3 , and
0.3-1.4 mg/m3 respectively during March-April 2018, and 3 to
34 μg/m3 , 8 to 88 μg/m3 , 53-256 μg/m3 , 2-121 μg/m3 and 34-
191 μg/m3 0.2-1.3 mg/m3 during October-November 2019. The
overall range of trace gases and particulate matter is consis-
tent with the mean values of these trace gases and partic-
ulate matter in 2018 and 2019 reported in Harbin, Xinjiang,
Yangtze River Delta region (Li et al., 2020a; Qin et al., 2021;
Sulaymon et al., 2021; Rupakheti et al., 2021).
Table 2 represents China National Air Quality Standards for
various criteria pollutants. The daily mean PM2.5 concentra-
tions exceeded the China National Air Quality Standard Grade
1 on about 68% and 48% of the observation days during 2018
and 2019. For PM10 , the concentration exceeded about on 92%
and 62% days for 2018 and 2019 respectively for Grade 1 China
National Air Quality standards. The daily mean SO2 concen-
trations did not exceed from the prescribed standards. The
661
overall reduction in SO2 levels can be linked to the strong and
effective measures taken to reduce the SO2 level. The previous
studies reported a decrease in industrial SO2 emissions fol-
lowing the widespread installation of fuel gas desulfurization
(FGD) devices in China (Li et al., 2020a; Rupakheti et al., 2021;
Zhang et al., 2017b). The daily mean NO2 concentrations did
not exceed from the prescribed standards. The daily mean O3
concentrations exceeded the China National Air Quality Stan-
dard Grade 1 on about 63% and 67% of the observation days
during 2018 and 2019. The previous studies also reported that
concentration of particulate matter and trace gases in differ-
ent pars of China exceeded the WHO guidelines and China Na-
tional Air Quality Standards (Li et al., 2020a; Rupakheti et al.,
2021).
The relationship between in-situ measurements and MAX-
DOAS observations for NO2 and SO2 is shown in Fig. 3. It is evi-
dent that both the observations are in good agreement depict-
ing a correlation coefficient (R2 ) of 0.60 and 0.61 for NO2 and
SO2 respectively at 0.05 significant level (2-tailed), thereby af-
firming the validity of the observations made by MAX-DOAS
instrument. It is worth to mention that as MAX-DOAS obser-
vations are made during sunlight. Therefore, the data of same
time period was used to investigate the relationship between
the in-situ measurements and MAX-DOAS observations
Despite the inability of MAX-DOAS instrument to detect
atmospheric species near the ground, the retrieval of trace
662 journal of environmental sciences 135 (2024) 656–668

Table 2 – Comparison of the mean concentration of different pollutants with the available guidelines/standards.

Parameters China This study (mean)

Grade 1 Grade 2 (March-April 2018) (Sept.-Oct. 2019)

PM10 50 150 118 83

PM2.5 35 75 54 40
SO2 50 150 22 12
NO2 80 80 32 37
O3 100 160 124 133

Fig. 3 – Correlation between MAX-DOAS observed VCDs of a) NO2 and b) SO2 with the in-situ measurements.

gas species at lower level provides with a reliable and robust
measurements of surface concentrations and trends of atmo-
spheric species. The concentrations of trace gas species in-
cluding NO2 and SO2 are normally concentrated in the lower
atmosphere, usually below 300 m, the concentrations can be
found consistent with the VCDs. Therefore, the influence of
near surface emissions on air pollution can be discussed us-
ing VCDs (Hong et al., 2019).
2.2. Complex pollution episodes
The higher concentrations of O3 and PM2.5 have adversative
effects on community health and the environment (Yue et al.,
2017). The complex pollution episode is basically the co-
occurrence of both PM2.5 and MDA8 O3 at higher levels. The
complex pollution days in this study refer to the pollution
conditions where the daily mean PM2.5 concentration exceeds
35 μg/m3 , and the daily mean O3 concentration exceeds 160
μg/m3 on the same day. The results depict that 20% of the
observation days in 2018 are identified as complex pollution
days, while during 2019, 21% of the observation days are found
to be complex polluted days. The previous studies also re-
ported the occurrence of the complex pollution episodes in
different regions of China recently (Lv et al., 2021; Qin et al.,
2021; Yue et al., 2017). It is evident from literature that com-
plex pollution episodes mostly occur during spring and au-
tumn seasons (Qin et al., 2021). Table 3 shows the mean values
of trace gases, particulate matter and meteorological parame-
ters during two different complex pollution episodes. The typ-
ical values of temperature, relative humidity and wind speed
ranges from 14-28◦ C, 53%-79% and 1.5-5.3 m/s respectively.
The study conducted in southern China reported that dur-
ing summer days when air temperature is high, the corre-
lation between PM2.5 and O3 was found strongly positive.
The other studies also reported that complex pollution of
PM2.5 and O3 was observed during days with relatively higher
temperature, relatively high RH, and lower wind speed. Ele-
vated temperature promotes O3 as well as sulfate formation
(Liao et al., 2009), higher RH favor the hygroscopic develop-
ment of PM2.5 and its corresponding constituents (Tie et al.,
2017), and dilution of pollutants in the atmosphere is dis-
couraged by lower wind speed. Lv et al. 2021 reported that
higher complex pollution hours (co-occurrence of both PM2.5
and MDA8 O3 at higher levels) were observed in Shanghai a
coastal city as compared to other in land cities e.g., Hefei,
which is likely because the sea-land breeze convergences
cause accretion of hourly O3 and PM2.5 in coastal areas. The
current study also reported frequent occurrence of complex
 journal of environmental sciences 135 (2024) 656–668
Table 3 – Comparison of the mean (standard deviation) concentration of different pollutants and meteorological parameters
during two complex pollution episodes.
Parameter (mean) Case 1 (23-28 March 2018)
3
PM2.5 (μg/m ) 93(24)
NO2 (μg/m3 ) 54(17)
O3 (μg/m3 ) 159(24)
SO2 (μg/m3 ) 30(5)
PM10 (μg/m3 ) 173(18)
CO (mg/m3 ) 1(0.1)
Temp (◦ C) 18(3)
RH (%) 58(8)
Wind speed (m/s) 3(1)
pollution episodes during March-April 2018 and September-
October 2019 in Dongying, a coastal city of Shandong province.
The atmospheric oxidation capacity Ox (O3 + NO2 ) for com-
plex pollution days is compared with other days of the ob-
servation. The results are indicative that higher oxidation ca-
pacity is observed during complex pollution days. The higher
oxidation capacity can increase the rate of formation of sec-
ondary pollutants. The similar results were reported in previ-
ous studies (Lv et al., 2021).
2.3. Ozone formation sensitivity
O3 formation in the atmosphere can be broadly categorized
into three distinct regimes: a) VOC-limited where VOC con-
centration determines O3 concentration, b) NOx limited where
the concentrations of NOx limit O3 formation, and c) transi-
tion regime where both VOCs and NOx play a role towards O3
formation (Hong et al., 2022). HCHO is the most abundant VOC
and NO2 constitutes major portion of NOx. Therefore, the ra-
tio of HCHO/NO2 (RFN) has been employed by various stud-
ies to assess the O3 -NOx-VOC sensitivity (Hong et al., 2022;
Xue et al., 2022; Zhang et al., 2021) where RFN less than 1
corresponds to VOC–limited regime, RFN more than 2 char-
acterizes NOx–limited regime, while an RFN value between
1 and 2 corresponds to transition regimes (Duncan et al.,
2010). Fig. 4 shows the daily mean RFN based on secondary
HCHO for Dongying. During March-April 2018, O3 formation
predominantly remained to be VOC-limited (52%) followed
by transitional (33%) and NOx-limited (15%) regimes. Dur-
ing September-October 2019, no contribution of NOx was ob-
served towards O3 formation in Dongying while both VOC-
limited and transitional regime had significant contribution of
55% and 45% respectively. These results imply that concurrent
control of both NOx and VOCs would benefit in ozone reduc-
tions.
Various studies conducted using MAX-DOAS observations
for O3 -NOx-VOCs sensitivity have been reported over differ-
ent parts of China in different seasons and are summarized
in Table 4. Our results are consistent with the studies con-
ducted over these regions. Near surface O3 sensitivity pre-
dominantly remained to be in VOC-limited regime for all the
seasons. Luo et al. (2020) classified the observation period
into clear and polluted days, reporting mixed sensitivity sce-
nario on clear days and VOC-limited in polluted days. How-
663
Case 2 (6-9 September 2019)
53(9)
25(8)
224(26)
11(0.8)
100(14)
1(0.1)
26(1)
66(2)
5(2)
ever, Tan et al. (2018) found O3 concentrations in ECS and YRE
to be NOx limited attributed to ship emissions. A difference
of 11.40% and 10% during March-April 2018 and September-
October 2019 respectively in O3 sensitivity was found between
HCHOtotal /NO2 and HCHOsec / NO2 . The results are indication
that primary HCHO have significant contribution in HCHO.
Therefore, the study of O3 sensitivity based on secondary
HCHO is crucial. A diurnal shift in O3 sensitivity was observed
from VOC-limited during the morning hours to VOC-NOx lim-
ited in the afternoon. The previous studies also reported in-
crease in O3 concentration during noon time while the O3 sen-
sitivity correspondingly shifted from VOC-limited to VOC-NOx
limited.
2.4. Diurnal variations
The variation in pollutant concentrations through the day
varies significantly depicting a peculiar diurnal trend specific
to each pollutant. This is because of the variability in emission
sources at different parts of the day as well as meteorological
parameters including solar radiation and other meteorologi-
cal parameters (Wang et al., 2013). The mean diurnal varia-
tions in the concentrations of species as observed by MAX-
DOAS instrument during March-April 2018 and September-
October 2019 are shown in the Fig. 5. The trend depicts that
NO2 concentration was higher during the morning hours at-
tributed to low solar intensity and more anthropogenic activ-
ity especially vehicle influx during the morning (Wang et al.,
2014; Kumar et al., 2015) and began to decline during the
day. This drop is linked to the increase in solar intensity
during the day which enhances photolytic reactions that act
as major sinks (Kumar et al., 2015). The concentration be-
gins to rise in the afternoon owing to the influx of traffic
during evening rush hours. Similar diurnal trend has been
observed for SO2 which has sources and sinks similar to
that of NO2 . Additionally, higher concentrations of pollutants
during the morning and evening hours might be related to
lower PBL during these hours, whereas, the PBL is raised
during the day time which allows for more diffusion and
thereby reduced concentrations in lower level (Pancholi et al.,
2018). HCHO depicts opposite diurnal trend implying the sec-
ondary sources of formation especially by the oxidation of
VOCs during the daytime (Gratsea et al., 2016; Chan et al.,
2019), thereby depicting a higher concentration during the
664 journal of environmental sciences 135 (2024) 656–668

Fig. 4 – Daily averaged RFN based on secondary HCHO showing O3 sensitivity to its precursors during March-April 2018 and
September- October 2019.

Table 4 – Overview of O3 -NOX -VOCs sensitivity over different regions of China.

Reference Study Location Study Period Study Season Study Findings

Chi et al., 2018 University of Chinese October 26 - November Autumn VOC-limited up to 700m,
Academy of Sciences, 6, 2014 Transitional from 700m to
Beijing 1km
Tan et al. (2018) East China Sea (ECS) and June 2 - 29, 2017 Summer NOx-limited
Yangtze River Estuary (YRE),
Shanghai
Zeng et al. (2018) Wuhan August 1 - 31, 2016 Summer VOC-limited
He et al. (2019) Heshan, Guangzhou October 22 - November Autumn VOC-limited
20, 2014
Luo et al. (2020) Jinan University Site, September 20 - Autumn Transitional under clear
Guangzhou November 20, 2018 conditions, VOC-limited on
polluted days
Zhang et al. (2021) Dianshan Lake, Qingpu October 17 - November Autumn VOC-limited within the
District, Shanghai 20, 2019 boundary layer
Hong et al. (2022) Guangzhou institute of July- September, 2019 Summer/Wet Season VOC-limited near surface,
Geochemistry, Chinese transitional between 0.4 -
Academy of Sciences 1.6km, VOC-limited above
1.6km
Xue et al. (2022) Liaoning University, January - November, Almost Year round VOC-limited
Shenyang 2019

day while lower concentrations during morning and evening
hours.
2.5. Correlation among criteria pollutants and
meteorological parameters
In order to study the correlation among the daily mean
meteorological parameters and criteria pollutants including
PM2.5 , PM10 , NO2 , SO2 , O3 , and CO the daily mean concen-
trations of these atmospheric species from the in-situ mea-
surements were utilized. The analysis was performed using
pairwise pearson’s correlation coefficient over the study area
and has been given in Fig. 6. During both the studied peri-
ods (March-April, 2018 and September-October 2019) PM2.5 de-
picted strongly positive correlation with PM10 , NO2 , and CO,
whereas for SO2 the correlation is strong for 2018 and mod-
 journal of environmental sciences 135 (2024) 656–668 665

Fig. 5 – Diurnal cycle of a) HCHO, b) NO2 and c) SO2 at elevation angle 2°.

Fig. 6 – Pearson Correlation between daily mean concentration of trace gases, particulate matter and meteorological
parameters (temperature and relative Humidity).

erate during 2019. With O3 , PM2.5 depicted weak correlation
for both the periods. The correlation between other species
were also found to be strong for both the studied periods ex-
cept for O3 which depicted moderate correlation with PM10 ,
SO2 , and NO2 during 2018 while weak correlation was ob-
served during 2019 especially with NO2 . Strong correlations
among the pollutants indicate similar sources of emission for
the pollutant species which may include the emissions from
automobiles and burning of fossil fuel. Our results are con-
sistent with the studies reported earlier (e.g., Sulaymon et al.,
666 journal of environmental sciences 135 (2024) 656–668
2021). It is worth mentioning here that the positive correla-
tion of PM2.5 observed with NO2 and SO2 is majorly accred-
ited to huge traffic emissions and power plants that utilize
coal as a major source of fuel (Zhang et al., 2020). Further, the
positive correlation of PM with major primary gaseous pollu-
tants (SO2 and NO2 ) might arguably be because these species
act as precursor for PM formation, especially sulfate and ni-
trate components (Li et al., 2021). The relatively weaker cor-
relation of O3 with other species reinforce that O3 formation
over the studied area is mostly VOC-limited. These results
reaffirm the previously reported conclusions (Sulaymon et al.,
2021). The results shown moderate positive correlation of tem-
perature with particulate matter in spring 2018 while dur-
ing autumn 2019 temperature shows weak positive correla-
tion with particulate matter. The temperature shows moder-
ate positive correlation with NO2 , SO2 and CO during spring
2018, while in autumn 2019 temperature shows weak cor-
relation with NO2 and SO2 . However, O3 shows strong posi-
tive correlation with temperature during spring 2018 and au-
tumn 2019. The rate of formation of O3 is higher when tem-
perature increases, as photolytic activity is increased which
helps in the formation of secondary pollutant O3 (Chen et al.,
2019; Li et al., 2020b). The relative humidity shows weak
to moderate negative correlation with particulate matter
and different trace gases during spring 2018 and autumn
2019.
3. Conclusion
This study was conducted over the city of Dongying in Shan-
dong Province of China. MAX-DOAS and in-situ observations
were used to monitor air quality of the city for two distinct
time periods, i.e., 9th March 2018 to 25th April 2018 and 1st
September to 30th October 2019. It is worth mentioning here
that mean concentrations for NO2 and SO2 remained signifi-
cantly below the acceptable national and international stan-
dards. However, both PM2.5 , and PM10 were observed to be
higher than the prescribed safe levels. The correlation coef-
ficient (R2 ) between the MAX-DOAS observations and in-situ
measurements for SO2 and NO2 was found to be 0.60 and 0.61
respectively, indicating that both the observations are in good
agreement and affirming the validity of MAX-DOAS instru-
ment. RFN indicates that the O3 production over Dongying lies
mostly in the VOC-limited region. The primary HCHO have
significant contribution in total HCHO. Therefore, the study
of O3 sensitivity based on secondary HCHO is crucial. A diur-
nal shift in O3 sensitivity was observed from VOC-limited dur-
ing the morning hours to VOC-NOx limited in the afternoon.
These results imply that concurrent control of both NOx and
VOCs would benefit in ozone reductions. The diurnal pattern
of HCHO showed an increase in concentration from morning
to noon and a reduction occurred afterward in the evening.
NO2 showed a prominent diurnal cycle peak in morning rush
hour followed by a decline towards noon and then a gradual
increase during evening. Similar to NO2 , SO2 concentrations
are higher during morning and evening hours, suggesting sim-
ilar sources of emission. Strong positive correlation was ob-
served between PM (PM10 and PM2.5 ), SO2 and NO2 while these
all species had weak correlation with O3 confirming that the
formation of O3 is linked to VOCs.
Declaration of competing interest
The authors declare that they have no known competing fi-
nancial interests or personal relationships that could have ap-
peared to influence the work reported in this paper.
Acknowledgments
This study was supported by the Jiangsu Funding Program
for Excellent Postdoctoral Talent (Grant No. 2022ZB651), the
National Natural Science Foundation of China (Grant No.
32071521), the Scientific Research Foundation for Senior Tal-
ent of Jiangsu University, China (Grant No. 20JDG067), the
Jiangsu Province “Double Innovation PhD” Grant.
Supplementary materials
Supplementary material associated with this article can be
found, in the online version, at doi:10.1016/j.jes.2022.09.014.
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