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Atmospheric Environment 246 (2021) 118152

Contents lists available at ScienceDirect

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

Characterization of black carbon aerosol at the summit of Mount Tai (1534


m) in central east China: Temporal variation, source appointment
and transport
Lijuan Shen a, Honglei Wang a, b, *, Xiangchen Kong c, Yan Yin a, Kui Chen a, Jinghua Chen a
a
Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Key Laboratory for Aerosol-Cloud-Precipitation of China Meteorological
Administration, Nanjing University of Information Science &Technology, Nanjing, 210044, China
b
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing,
100029, China
c
Ordos Meteorological Bureau of Inner Mongolia, Ordos, 017000, China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• BC was measured at the summit of Mt.


Tai.
• A significant diurnal variation in BC,
BCliquid and BCsolid was observed.
• BCliquid to total BC was 64.7% at the
summit of Mt. Tai.
• Long-range transport from the YRD re­
gions contributed 2000 ng m− 3 to BC in
summer at Mt. Tai.
• Air masses passing through Mt. Tai
contributed more than 1800 ng m− 3 to
BC in the whole NCP region.

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

Keywords: As a crucial absorption component of aerosols, black carbon (BC) plays a key role in modifying aerosol-planetary
BC boundary layer (PBL) meteorology and hence aggravating haze pollution. With an altitude of 1534 m, Mt. Tai is
Source appointment close to the top of the PBL and located within the transportation channel from the North China Plain (NCP) to the
Concentration weighted trajectory (CWT)
Yangtze River Delta (YRD). In this study, BC aerosols were continuously observed using a seven-channel
Regional transport
aethalometer (AE-33) at the summit of Mt. Tai from May 11 to June 25, 2017. The temporal variation, source
and transport characteristics of BC in the upper PBL of central and eastern China in summer were then discussed.
The average concentrations of BC, BCliquid and BCsolid were 1722.6, 1194.6 and 545.8 ng m− 3, respectively,
during the observation period. Liquid fuel sources were calculated and accounted for 64.7% of the BC mass
concentration. The distributions of BC were mostly centralized in concentrations less than 600 ng m− 3 (ac­
counting for 21.9% of the total BC samples) and ranged from 1400 to 2200 ng m− 3 (32.5%). Meteorological
elements were determined to have great impacts on the distribution of BC concentrations, which increased with
the decrease in visibility and wind speed and the increase in relative humidity (RH). The diurnal variations in BC
presented high values during the daytime and low values during the nighttime, with peaks at 06:00, 11:00 and
18:00. Long-range transport from the YRD regions in summer, as well as the surrounding regions, played an

* Corresponding author. Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Key Laboratory for Aerosol-Cloud-Precipitation of
China Meteorological Administration, Nanjing University of Information Science &Technology, Nanjing, 210044, China.
E-mail address: hongleiwang@nuist.edu.cn (H. Wang).

https://doi.org/10.1016/j.atmosenv.2020.118152
Received 3 April 2020; Received in revised form 30 November 2020; Accepted 14 December 2020
Available online 16 December 2020
1352-2310/© 2020 Elsevier Ltd. All rights reserved.
L. Shen et al. Atmospheric Environment 246 (2021) 118152

important role in determining the BC concentrations at Mt. Tai with concentration weighted trajectory (CWT)
values exceeding 2000 ng m− 3. Air masses may move northward to the NCP after passing through Mt. Tai, and
they contributed more than 1800 ng m− 3 to the BC in the whole NCP region.

1. Introduction Guwahati. In Milan, Italy, Mousavi et al. (2019) studied BC in urban sites
mainly originating from fossil fuels, and suburban sites had significantly
By absorbing or scattering solar radiation, atmospheric aerosols can higher biomass burning.
change temperature distributions, leading to an alteration of the struc­ With an altitude of 1534 m, Mt. Tai is the highest mountain in central
ture of the aerosol-planetary boundary layer (PBL) (Li et al., 2017). As a and eastern China and is at the top of the PBL height. A number of
crucial absorption component of aerosols, black carbon (BC) can lower studies have recently been carried out in the NCP and Yangtze River
the PBL height by heating the upper PBL, resulting in the aggravation of Delta (YRD) as regions with complex pollution (Gao et al., 2016; Ji et al.,
haze pollution (Ding et al., 2016; Huang et al., 2018; Wang et al., 2015). 2019; Liu et al., 2020; Tang et al., 2016; Wang et al., 2020). Significant
A related study reported that light-absorbing aerosols such as BC can transport of air pollutants occurs between these two regions due to the
change the maximum temperature in the upper PBL by approximately impacts of terrain and atmospheric circulation (Kang et al., 2019). Mt.
0.7 ◦ C on average in pollution processes (Huang et al., 2018). Tai is located within the transportation channel from the NCP to the
BC aerosols mainly originate from incomplete combustion of fossil YRD. Therefore, a continuous investigation of BC at Mt. Tai can enhance
fuel and biomass; the former includes vehicle exhaust and coal burning, our knowledge of the cross-region transport mechanism of air pollutants
and the latter refers to straw and wood burning and waste incineration to regulate regional air quality. In this study, BC aerosols were contin­
(Bond et al., 2004; Gertler et al., 2016; Ni et al., 2014; Wang et al., uously observed at the summit of Mt. Tai from May 11 to June 25, 2017,
2014). Bond et al. (2004) calculated that the global BC emissions were by using the seven-channel aethalometer (AE-33). The distribution,
~8.0 t g in 1996 according to PKU-BC-2007, and the global total and source and transport characteristics of BC were then discussed by using
anthropogenic BC emissions in 2007 were 8.9 and 6.3 Tg, respectively, the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT),
among which Asia contributed 4.1 Tg to the total and 3.8 Tg to the the potential source contribution function (PSCF) and concentration
anthropogenic BC. With the fastest developing economy in the world, weighted trajectory (CWT) models.
China has suffered sharp increases in air pollutants (Wang et al., 2014).
The total BC emissions from China in 2007 were estimated to be 963.4 2. Experiments and methods
Gg (Ni et al., 2014). Related studies estimate that BC emissions in China
are 1224.4 Gg in 2020 (Streets et al., 2001) and are predicted to be 2.1. Description of the observation site
920–2183 Gg/yr under various scenarios in 2050 (Wang et al., 2012).
BC can only be removed from the air by dry and wet deposition The sampling site was located at the weather station on Sun Viewing
processes due to its stable chemical properties, which result in its Peak on Mt. Tai (36.25◦ N, 117.10◦ E; 1534 m). The observation time was
longevity in the air for several days to weeks; BC can therefore undergo from May 11 to June 25, 2017. Mt. Tai, with a total area of approxi­
long-range transport processes (Chen et al., 2016; Hvidtfeldt et al., 2019; mately 426 km2, is located 6 km north of the city of Tai’an and
Ni et al., 2014). Regional compound pollutants have been increasingly approximately 60 km south of the provincial capital Jinan. Mt. Tai
serious in central and eastern China due to the high levels of urbaniza­ stretches over Tai’an, Jinnan, and Zibo and is ~200 km in the east-west
tion and population density (Mao et al., 2019; Xu et al., 2019). BC direction and ~50 km in the south-north direction. Being 430 km from
concentrations are capable of increasing sharply during haze episodes, Beijing, 500 km from Nanjing and 68 km from Shanghai, Mt. Tai is
leading to a rapid decrease in visibility. Chen et al. (2017) discovered located within the transportation channel from the NCP to the YRD. The
that the increase in BC absorption was primarily associated with AOD values were high over Central and Eastern China during the
urban-scale photochemical production of nitrate and sulfate aerosols observation period (Fig. 1). Hence, the local and regional emissions
during the haze pollution process. Wang et al. (2016) reported that the substantially contribute to the air quality at the summit of Mt. Tai. Mt.
average mass concentration of BC was 6.1 ± 3.9 μg m− 3 during hazy Tai’s altitude is close to the top of the PBL over central and eastern
periods, which was 4.7 times higher than that during non-hazy periods China, and local cloud events frequently occur at its summit, especially
in Beijing. Moreover, by using the SP2 to vertically measure the BC in summer.
during a haze episode in the winter of 2018 in Beijing, it was found that
BC particles were significantly coated with mass ratio of coating over 2.2. Description of observation instruments
refractory BC increasing from about 1 to 10, the coatings on the surface
of BC may introduce an additional heating rate as high as 0.1 K/h on The BC mass concentration was observed with a Model AE-33
hazy days (Zhao et al., 2020)Zhao et al., 2020. aethalometer (Magee Scientific, USA). This aethalometer uses two-
BC can also be used as a tracer to study the regional transport point measurement technology and dynamic zero-point calibration to
mechanism due to its stable properties (Moteki et al., 2012; Parungo provide continuous observations at fixed points at seven wavelengths
et al., 1994; Sharma et al., 2013; Shores et al., 2013; Wang et al., 2016). (370, 470, 520, 590, 660, 880, and 950 nm). The BC concentrations
Wang et al. (2016) observed that 71.4–82.0% of the BC in Beijing was reported in the present study were measured using the AE-33 that is
from regional transport during high BC episodes and that 47.9–56.8% of described in great detail elsewhere ( Jing et al., 2019; Zhang et al.,
the BC can be attributed to sources on the central North China Plain 2017). The PM2.5 and PM10 concentrations were measured with sensors
(NCP). Aruna et al. (2013) found that the BC concentration showed from the LGH-01 E and LGH-01 B Landun Photoelectron Company.
significant diurnal variation only during the northeastern monsoon in Meteorological data, such as wind speed/direction, temperature, pres­
Chennai, India. Numerous studies have investigated the source charac­ sure, relative humidity, visibility and precipitation, were obtained from
teristics of BC as well (Barman and Gokhale, 2019; Briggs and Long, a CSI-CR1000 automatic weather station.
2016; Hegg et al., 2009; Helin et al., 2018; Mousavi et al., 2018). Liu
et al. (2018) reported that burning solid fuels, including coal and
2.3. Absorption ångström exponent (AAE)
biomass, were dominant factors in BC during haze episodes in Beijing.
Barman and Gokhale (2019) discovered that emissions of BC from ve­
The absorption coefficient babs (λ) (Mm− 1) of carbonaceous aerosols
hicles increased by 62% from 2011 to 2018 in the northeastern city of
was derived from the following formula (Drinovec et al., 2015):

2
L. Shen et al. Atmospheric Environment 246 (2021) 118152

where AAEliquid and AAEsolid represent the aerosol absorption Ångström


exponent of BC generated from liquid and solid fuels, respectively, and
MAC represents the BC mass absorption cross-section. BCsource comprises
sources of liquid and solid fuels; P represents the percentage of BC from
liquid fuels to the total BC.

2.5. MODIS AOD

MODIS is a detector mounted on the Terra and Aqua satellites of the


EOS. In this study, Terra MODIS C6.1 Level 3 aerosol products
(MOD08_D3) at 1 ◦ × 1 ◦ were used, and data were downloaded from the
NASA Level 1 and Atmosphere Archive and Distribution System (http
s://ladsweb.modaps.eosdis.nasa.gov/search/order/1). The dark target
and deep blue merged aerosol optical depth (AOD) data at 550 nm
(hereafter referred to as AOD) were principally used in this study. The
details of the MODIS can be found in Qin et al. (2018).

2.6. NCEP/NCAR reanalysis data

NCEP/NCAR Reanalysis Products-1 (NNRP-1) data was produced by


the National Centers for Environmental prediction (NCEP) in collabo­
ration with the National Centre for Atmospheric Research (NCAR) and it
covers the period from 1948 to present day. The data assimilation sys­
tem uses a 3D-variational analysis scheme, with 28 sigma levels in the
vertical and a triangular truncation of 62 waves. A forecast from the
Fig. 1. Distributions of MODIS AOD in May and June. NCEP global spectral model was used as the first-guess fields for this
reanalysis. The assimilation system used in NCEP/NCAR reanalysis is
babs (λ) = BC(λ) × MAC(λ) described in more detail in Kalnay et al. (1996). Here, we used the
reanalysis data during the observation period in 2017 and over the same
where BC(λ) refers to the mass concentration of BC at different wave­ period during 2000–2016 to calculate the climatological wind field,
lengths and MAC(λ) refers to the mass absorption cross section. which were all provided by the NCEP (https://www.ncep.noaa.gov/),
The relationship between babs (λ) and the wavelength λ for carbona­ with a horizontal resolution of 1 ◦ × 1 ◦ .
ceous aerosols is expressed as follows:

babs(λ) = K × λ− AAE 2.7. HYSPLIT model

where λ is the light wavelength, K is a constant, and AAE represents the Air mass backward trajectories for 24 h at 500 m above the obser­
aerosol absorption Ångström exponent. The absorption coefficients of 7 vation sites were simulated every hour by the Hybrid Single-Particle
wavelengths were used to fit the exponential function curve to obtain Lagrangina Integrated Trajectory (HYSPLIT) model (http://ready.arl.
the AAE values. noaa.gov/HYSPLIT.php), which was developed by the National
Oceanic and Atmospheric Administration (NOAA) Air Resources Labo­
ratory (ARL). The model has been widely used in the study of air
2.4. Aethalometer model pollutant transport (Stein et al., 2015). The National Weather Service’s
National Centers for Environmental Prediction (NCEP) Global Data
The Aethalometer model is based on the work of Sandradewi et al. Assimilation System (GDAS) archive was used for meteorological input
(2008) and aims to quantify the contribution of fossil fuel (BCff) and data, with a horizontal resolution of 1.0 ◦ × 1.0 ◦ .
biomass burning (BCbb) to the total BC mass concentration. Zhang et al.
(2009) \discovered that the BC emitted in China originates mainly from
liquid and solid fuels. The total light absorption at 880 nm was therefore 2.8. Potential source contribution function (PSCF) models
ascribed to the BC from liquid fuels (vehicle exhaust) and solid fuels
(coal and biomass burning) (Jing et al., 2019). Consequently, The PSCF, developed by Aruna et al. (2013), has been widely used in
several research domains (Lucey et al., 2001; Wang et al., 2016; Xu et al.,
babs(BC) = babs(BCliquid) + babs(BCsolid)
2019). A single grid cell was calculated by counting each trajectory
segment endpoint that terminated within that grid cell. The number of
babs(370nm)liquid 370 −
endpoints (higher than an arbitrarily threshold value) that fell in a
AAEliquid
=( )
babs(880nm)liquid 880
certain grid (i, j) at a time was marked as mij , while the total number of
babs(370nm)solid 370 − endpoints that fell in the same grid cell was denoted as nij . Therefore, the
AAEsolid
babs(880nm)solid
=(
880
) PSCF was defined as:
mij
PSCFij =
babs(880nm)source nij
BCsource =
MAC(880nm)
To remove the uncertainty in the cells with small values of nij, an
babs(880nm)liquid BCliquid arbitrary weight function Wij was multiplied by the PSCF values to better
P=
babs(880nm)
=
BC reflect the uncertainty in the values for these cells (Polissar et al., 2001;
Wang et al., 2009), so the weight function W(nij ) was defined as:

3
L. Shen et al. Atmospheric Environment 246 (2021) 118152

1.0 , 120 < nij m− 3 and 20.6 μg m− 3. A good correlation was found between BC and
0.8 , 40 < nij ≤ 120 PM2.5, with a correlation coefficient of 0.65.
W(nij ) = {
0.4 , 20 < nij ≤ 40 The AOD shown high values over the Central and Eastern China
0.2 , nij ≤ 20 during the observation period (Fig. 1). Particularly, the AOD values
exceeding 0.8 were noticed in the NCP and YRD, which were located at
and then, the WPSCFij was derived based on the following formula: the north and the south of Mt. Tai, respectively. Whereas, the wind fields
mij at 850 hPa during the observation period in 2017 were generally the
WPSCFij = × W(nij )
nij same to the climatological wind fields over 2000–2016 (Fig. 3). The
southwesterly winds dominated over Mt. Tai attributing to the impacts
of subtropical high pressure, which also revealed stable meteorological
2.9. Concentration weighted trajectory (CWT) model conditions over CEC. Additionally, such prevailing southerlies also
suggested the pollutant transport from south directions, the YRD for
PSCF can only reflect the proportion of polluted trajectories in a instance, where the aerosol pollution was significant (Fig. 1).
certain grid, while it cannot calculate the concentration contribution of The wind speed varied sharply, with a maximum value of 21.2 m s− 1
the polluted trajectories to a target grid cell. Therefore, the CWT, and an average of 6.1 m s− 1. Large winds generally corresponded to low
assigning the average weighted concentration associated with each concentrations of PM2.5 and BC. At the same time, the RH varied
trajectory to the grid cells, was used with the aim of producing a intensively due to the local cloud-fog process, e.g., the RH was 17.5% at
geographical overview of emissions source areas (Hsu et al., 2003): 14:00, May 11, and increased to 58.0% 3 h later. As a result, the RH
ranged from 9.6% to 100.0%, with an average of 66.2%. The visibility
1 ∑
M
Cij = ∑M Ck τijk had the opposite variation pattern to that of RH, a correlation coefficient
τ
k=1 ijk k=1 of − 0.82 was found between them, and hence, high visibility occurred at
Mt. Tai with an average of 18.3 km and a maximum value of 35 km.
where Cij is the average weighted concentration in theijcell, k is the Strong precipitation processes frequently occurred at the summit of
index of the trajectory, M is the total number of trajectories, Ck is the Mt. Tai, as shown in Fig. 2. Generally, the PM2.5 and BC concentrations
concentration observed on arrival of trajectory k in the ij cell, and τijk is were low when precipitation was accompanied by high wind speeds.
the time spent in the ij cell by trajectory. The weight function Wij was However, the BC values were relatively high between 10:00–13:00 on
also applied to the CWT analysis to reduce the uncertainty in the cells June 21 when a strong rainfall occurred; the decrease in BC concen­
with small values ofnij : trations began just after the termination of this rainfall, which revealed
WCWTij = Cij × W(nij ) that the precipitation process may carry foreign pollutants to Mt. Tai.
Fig. 4 shows that the BC frequency had bimodal distributions peak­
ing at values smaller than 600 ng m− 3 and between 1400 and 2200 ng
3. Results and discussion
m− 3, accounting for 21.9% and 32.5% of the total BC samples, respec­
tively. The BC frequency decreased rapidly with the increase in BC when
3.1. Overview
the BC concentrations were higher than 2200 ng m− 3. However, the BC
samples constituted 2.4% of the total samples when the BC concentra­
As shown in Fig. 2, the mass concentrations of BC and PM2.5 fluc­
tions ranged from 4400 to 6000 ng m− 3.
tuated greatly during the observation period. The BC and PM2.5 had
The variations in PM2.5 coincided with those in BC, and low PM2.5
hourly concentrations ranging from 1.7 to 5877.9 ng m− 3 and from 2 to
concentrations normally corresponded to low BC values. The PM2.5
97.9 μg m− 3, respectively, and the averages of which were 1722.6 ng

Fig. 2. Hourly changes of BC, PM2.5 and meteorological parameters during the observation period.

4
L. Shen et al. Atmospheric Environment 246 (2021) 118152

Fig. 3. Distributions of the 850 hPa wind fields (a) during the observation period in 2017 and (b) over the same period during 2000–2016.

Fig. 4. Frequency distribution of BC and the corresponding variations of PM2.5 and meteorological elements.

fluctuated greatly when the BC concentrations were high, e.g., the PM2.5 the summit of the mountains. While low wind speeds during the daytime
value was 75.5 μg m− 3 in the BC ranges of 4200–4400 ng m− 3 and promoted the accumulation of pollutants, high wind speeds during the
decreased to 21.4 μg m− 3 at BC values of 4800–5000 ng m− 3. On the one nighttime was ascribed to the high altitude of Mt. Tai making it in the
hand, the statistical error increased as the samples of high BC values free atmosphere, which favored pollutant diffusion combined with
decreased; on the other hand, local sources of BC, such as temple incense reduced human emissions.
burning and cooking processes, had larger impacts on BC concentrations Three peaks at 6:00, 11:00 and 18:00 were observed for BC due to the
than on PM2.5, which resulted in a great fluctuation in PM2.5 under high impacts of temple incense burning and cooking processes (Fig. 5a). The
BC conditions. visibility decreased to valley values once BC reached peak values.
The BC concentrations normally decreased with increasing visibility However, the maximum and minimum values of visibility were 20.0 ±
and wind speed and increased with increasing RH. However, the wind 12.7 km and 16.3 ± 13.1 km at 08:00 and 22:00, respectively, when the
speeds increased when the BC values exceeded 5200 ng m− 3, and under babs were 11.9 ± 7.9 Mm− 1 and 11.7 ± 8.9 Mm− 1 (Fig. 5c), revealing
these wind conditions, the wind speed and RH were revealed to have that the BC concentrations were not the main factor affecting the visi­
negative correlations with PM2.5 and visibility. The impacts of meteo­ bility at Mt. Tai.
rological conditions and emissions sources on BC and PM2.5 differed PM2.5 had similar diurnal variations to those of BC but had greater
under high BC conditions. fluctuations, as shown in Fig. 5b. PM2.5 sources were much more com­
plex than those of BC, and soil dust contributed greatly to PM2.5 when
the wind speed was high in where there was relatively lower vegetation
3.2. Diurnal variations in BC concentrations
cover at Mt. Tai, which resulted in a small PM2.5 difference between day
and night. Additionally, high RH, especially at night, was conducive to
Fig. 5 shows that the diurnal variations in BC presented high values
the formation of secondary components in PM2.5.
during the daytime and low values during the nighttime, which was due
The BC/PM2.5 ratios were also large, with an average of 11.8% ±
to the elevated PBL height favoring the upward transport of foreign
9.9% (Fig. 5d), and they began to increase from 11.7% ± 8.7% at
pollutants and intensive human emissions during the daytime. The wind
08:00–15.7% ± 11.4% at 10:00. Hereafter, they fluctuated until 19:00,
speed and temperature changed in contrast to and according to that of
with a value of 10.7% ± 7.8%, which reflected that BC was also greatly
BC (Fig. 6). High daytime temperatures may have increased the PBL
influenced by local emissions.
height, which was conducive to the delivery of surface pollutants up to

5
L. Shen et al. Atmospheric Environment 246 (2021) 118152

Fig. 5. Diurnal variations of BC, PM2.5, babs and BC/PM2.5 ratio.

Fig. 6. Diurnal variations of meteorological elements.

3.3. Source apportionment of BC by the aethalometer model abroad (Zotter et al., 2017). Related studies have indicated that AEEs
close to 1.1 represent the traffic sources (liquid fuels) of BC, 0.8–1.2
In this study, the Aethalometer model was used to quantify the represent fossil fuel burning, and 1.8–2.2 represent biomass combustion
contributions of different sources to BC mass concentrations, and this (Harrison et al., 2013; Olson et al., 2015; Sandradewi et al., 2008). In
model has been widely applied to source apportionment in China and China, coal and biomass are both important solid fuel sources of BC and

6
L. Shen et al. Atmospheric Environment 246 (2021) 118152

have identical AAE values in Beijing (Liu et al., 2018); therefore, we YRD regions mainly accounted for the BC, with few contributions by
considered coal and biomass as solid fuels for discussion. The linear surrounding areas.
relationship between AAE and P was derived to confirm the AAE values Fig. 9c and d shows that the backward CWT distributions of PM2.5
for liquid and solid fuels. As shown in Fig. 7, a noticeably negative and BC were similar, with high values located in Qingdao, Linyi, Jining,
correlation between AAE and P was observed with an R value equal to Zaozhuang and Heze of southern Shandong; Kaifeng, Shangqiu and
− 0.994. The AAE values were calculated to be 2.17 and 1.04 when P was Zhoukou of eastern Henan Province; Suzhou, Bozhou and Bengbu of
0 and 1, respectively; hence, we chose 1.04 for AAEliquid and 2.17 for northern Anhui; and Xuzhou, Suqian, Nanjing, Lianyungang and Yan­
AAEsolid in our study. cheng of Jiangsu, where the contributions exceeded 20 μg m− 3 PM2.5
The AAE and P values ranged from 0.56 to 2.38 and 0.3%–99.8% and were more than 2000 ng m− 3 of the BC mass concentrations at Mt.
during the observation period, with averages of 1.33 and 64.7%, Tai. High AOD values were also observed in these high CWT value re­
respectively, indicating the diverse and variable source strengths of BC gions, especially that of BC (Fig. 1). Regionally high AOD values were
emissions. Fig. 8 reveals that the AAE and P had contrasting diurnal observed in central and eastern China with no obvious boundary,
variations with high AAE values during the daytime. The AAE values identical to those of high CWT values of PM2.5 and BC representing the
used to identify the particle sizes and sources (Schuster et al., 2016) local and long-range transport of emission sources, respectively. How­
were close to 1, indicating fresh BC had small particle sizes and aging BC ever, there were still some discrepancies between the potential source
larger than 1.6 had large particle sizes, e.g., brown BC with strong contributions of PM2.5 and BC, and the high CWT values of BC were
wavelength dependency (Bond and Bergstrom, 2006; Lack and Cappa, more distributed in southwestern cities, such as Xuzhou, Bengbu, Suqian
2010). The AAE values were high at 05:00–10:00 with low P values, and Hefei, where high AOD values dominated as well. The eastern re­
suggesting large sizes of BC particles and a lower contribution by liquid gions of Mt. Tai, including the cities of Qingdao and Rizhao, contributed
fuels in this period than in the other periods. greatly to PM2.5 but little to the BC mass concentrations (Fig. 9).
The BCliquid and BCsolid concentrations had averages of 1194.6 and
545.8 ng m− 3, ranging from 0.6 to 5348.6 ng m− 3 and 0.7–3039.7 ng 3.4.2. Forward trajectory analysis
m− 3, respectively. Similar to the diurnal variations in BC, BCliquid had The potential impact areas of PM2.5 and BC were common, as shown
bimodal distributions (Fig. 8a), while BCsolid had a unimodal distribu­ in Fig. 10, generally located in NCP regions, which was contrary to their
tion (Fig. 8b). The BCliquid reached a maximum value of 1643.1 ± potential source distributions. High forward PSCF values of BC were
1048.8 ng m− 3 at 18:00, which was higher than the morning peak value found to have a wider range than that of PM2.5. PM2.5 with high forward
and probably occurred due to the large amounts of natural gas burning PSCF values was mainly distributed in Zibo, Dongyin, Weifang and the
(liquid fuels) at dinner time. The BCsolid concentrations began to in­ Bohai Sea, and the second transport pathway was located in Shangqiu,
crease at 05:00 and returned to a normal level at 19:00, the period of Kaifeng and Zhoukou. The air mass at Mt. Tai had three forward
which was in accordance with the temple incense burning activities that transport pathways: the first was similar to that of the PM2.5 distributed
accounted for the biomass combustion (solid fuels). The decrease in from Zibo, Dongyin and Weifang to the Bohai Sea; the second moved
BCsolid was followed by the decrease in human activities after 18:00, northward to Dezhou, Cangzhou, Tianjing and Tangshan with PSCF
with the largest rate drop of 130.9 ng m− 3⋅h− 1; hence, BCsolid returned to values larger than 0.9 in Tianjing and Tangshan; and the third was
a background level in 2–3 h. distributed in Shijiazhuang and Baoding.
The forward CWT distribution of PM2.5 was similar to that of PSCF,
mainly located at Zibo, Dongyin, Weifang and the Bohai Sea, with
3.4. PSCF and CWT contributions exceeding 24.0 μg m− 3 or even larger than 30.0 μg m− 3 in
the Bohai Sea. The NCP was also observed to have high CWT values,
3.4.1. Backward trajectory analysis including in Tianjing, Tangshan, Shijiazhuang and Baoding, with con­
The backward PSCF distributions of PM2.5 and BC differed, as shown tributions ranging from 18.0 to 24.0 μg m− 3, and in Shangqiu, Kaifeng
in Fig. 9 (a) and Fig. 9 (b), respectively. The PM2.5 had wider PSCF and Zhoukou, with contributions over 24.0 μg m− 3. Similar to the for­
ranges than those of BC with two high value areas. The first was ward PSCF distribution of BC, the forward CWT values of BC had three
distributed in the surrounding regions of Jinin, Linyi, Zaozhuang and high value centers as well, which were linked with contributions
Lianyungang, Kaifeng and Heze. The second, located in the YRD regions, exceeding 2000.0 ng m− 3. The whole NCP had high CWT values with
including Yancheng, Nantong and Shanghai, had a long-range transport large amounts of BC (>1800.0 ng m− 3).
contribution to PM2.5 at Mt. Tai. However, long-range transport from the The PM2.5 and BC at Mt. Tai were mainly affected by the surrounding
sources and the long-range transport of pollutants from YRD regions in
summer, and the air masses may have moved northward to NCP regions
after passing through Mt. Tai, which indicated a strong cross-region
transport of air pollutants. Therefore, the AOD values in central and
eastern China were generally high in summer, likely due to monsoon
impacts. Air pollutants transported northward from the YRD to the NCP
served the prevailing southerly wind in summer and contrary southward
from the NCP to the YRD in winter due to the control of cold high
pressure in central and eastern China. Therefore, the cross-regional
transport of air pollutants should be fully considered in regulations for
regional air quality.

4. Conclusions

In this study, BC aerosols were continuously observed at the summit


of Mt. Tai from May 11 to June 25, 2017, by using the AE-33 aethal­
ometer. The distribution, source and transport characteristics of BC in
the upper PBL of central and eastern China in summer were then dis­
cussed. The average concentrations of BC, BCliquid and BCsolid were
Fig. 7. Relationship between P and AAE values during the observation period. 1722.6, 1194.6 and 545.8 ng m− 3 during the observation period,

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L. Shen et al. Atmospheric Environment 246 (2021) 118152

Fig. 8. Diurnal variations of BCliquid, BCsolid, AAE and P.

Fig. 9. Backward trajectories of BC and PM2.5 by PSCF and CWT model.

ranging from 1.7 to 5877.9 ng m− 3, 0.6–5348.6 ng m− 3 and 0.7–3039.7 wind speed and the increase in RH. The diurnal variations in BC pre­
ng m− 3, respectively. Liquid fuel sources were calculated to contribute sented high values during the daytime and low values during the
64.7% to BC concentrations. The distributions of BC were mostly nighttime, with peaks at 06:00, 11:00 and 18:00. The BC/PM2.5 ratios
centralized in concentrations smaller than 600 ng m− 3 (accounting for fluctuated sharply with an average of 11.8% ± 9.9%. Long-range
21.9% of the total BC samples) and in the range of 1400–2200 ng m− 3 transport from the YRD regions in summer, as well as the surrounding
(32.5%). Meteorological elements were noticed to have great impacts on regions, played important roles in the BC and PM2.5 concentrations at
BC contributions, which increased with the decrease in visibility and Mt. Tai with contributions exceeding 2000.0 ng m− 3 and 20.0 μg m− 3,

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L. Shen et al. Atmospheric Environment 246 (2021) 118152

Fig. 10. Forward trajectories of BC and PM2.5 by PSCF and CWT model.

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