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Atmospheric Environment 272 (2022) 118966

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

Observational study of the PM2.5 and O3 superposition-composite pollution


event during spring 2020 in Beijing associated with the water vapor
conveyor belt in the northern hemisphere
Jizhi Wang a, *, Yuanqin Yang a, Xiaofei Jiang b, Deying Wang a, Junting Zhong a, Yaqiang Wang a
a
State Key Laboratory of Severe Weather and Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing, 100081, China
b
China Meteorological Administration Training Centre, Beijing, 100081, China

H I G H L I G H T S

• Special meteorological condition is resulting in composite pollution of PM2.5 & O3


• Interaction between water vapor transport & microphysical condensation is the key
• Daily cycling change of solar radiation supports composite pollution of O3 & PM2.5

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

Keywords: Unlike the heavy haze situations in previous years, the emergence of a water vapor conveyor belt flowing
Superposition-composite influence through North China is an important factor in the foggy-haze event during the 48-h snowfall in Beijing and its
O3 and PM2.5 surroundings, which disrupted the customary pollution snow removal atmospheric purification.
Super-saturation
①In the spring of 2020, during a period of negative emissions increment and weak human activity impact, a
Condensation
Water vapor conveyor belt
special interaction between the high humidity content of large-scale continuous water vapor transmission and
Power exponential law the weather-scale daily cycling radiation cycle change (due to daily change of sun’s zenith angle), as well as the
atmospheric microphysical process, provided rare meteorological conditions for the superposition-compound
growth of PM2.5 and O3 pollution. The water vapor conveyor belt, through enhanced transmission of easterly
wind momentum, induced a high value super-saturation signal (S) and condensation rate (fc), resulting in 48
consecutive hours of snow in Beijing, but was also conducive to fine particulates, including precursor emissions,
through a microphysical humidification process, which became synchronized. ②The weather-scale process
impact refers to the cloud height rise in the daytime and decrease at night. Due to the daily fluctuations in cloud
height, the concentration of O3 followed a coordinated daily cycle. During the day, when the sun’s zenith angle
going on the top, the PM2.5 and O3 superposition composite effects occur. Therefore, even during a negative
emission period, PM2.5 and O3 superposition-composite serious pollution events occur as usual, rather than the
expected possible atmospheric cleaning through snow.

1. Introduction air quality society-wide can occur during this time. However, from
February 10 to 14, 2020, Beijing, Tianjin, North China, and the sur­
Since February 2020, during the traditional Chinese Spring Festival roundings experienced a heavy pollution weather process, the formation
(SF) and the continuation of the long holiday, all relevant regions in mechanism of which has attracted much attention.
China experienced long vacations in which people stayed at home, cars As shown in Fig. 1 and Table 1, during the SF in 2020, the average
remained in parking lots, and factories closed on holidays, leading to emissions of PM2.5, SO2, NOx, and VOCs were lower than those before
negative emission increments. Therefore, a window period of excellent the SF and during the same period since 2017. Overall, the average

* Corresponding author. State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sci­
ences, China.
E-mail address: jzwang@cma.gov.cn (J. Wang).

https://doi.org/10.1016/j.atmosenv.2022.118966
Received 8 November 2021; Received in revised form 17 January 2022; Accepted 19 January 2022
Available online 7 February 2022
1352-2310/© 2022 Published by Elsevier Ltd.
J. Wang et al. Atmospheric Environment 272 (2022) 118966

2017) presented an article in Scientific Reports and several series of


articles, which suggested that through positive feedback loops caused by
aerosol–cloud interactions, further increase of both O3 and PM2.5 con­
centrations can be realized, which are partly responsible for the severe
PM2.5 pollution in China. In fact, due to the dynamic feedback of those
condensation-based microphysical meteorological conditions, the event
may re-intensify particulate concentration (Zhang et al., 2009, 2015,
2020; Zhong et al., 2018a). The substantial effects on synergistic con­
centration increase of O3 and PM2.5 could also be seen from the hu­
midification of particulate matter and cloud microphysical processes
(Sheng et al., 2017; Spracklen et al., 2008). Studies have indicated that
water vapor transport is a necessary condition for rain and snowy
weather, and this large-scale water vapor transport belt is closely related
to the temporal and spatial distribution of rainfall and snow (Zhu and
Newell, 1994).
Fig. 1. The decreasing characteristics of average pollution emission observed in
These heavy pollution observations coincide with a period of nega­
28 city points around Beijing, Tianjin, Hebei and surrounding during February
2020 comparing with the period before the Spring Festival as well as to the tive emissions increments, when human activity had no impact in
same period for the recent average since 2017. February 2020. Therefore, the long periods of heavy pollution during
snowfall in Beijing rather than anticipated snow removal of pollution
may hardly to be understood in this context.
Table 1 In this study, based on a comparative analysis of the effects of the
Emissions decrease of all type pollutants. large-scale water vapor transport belt in northern hemisphere, we
Emissions Before SF Since 2017 discuss the special formation mechanism of heavy pollution process
under the humidification of particulates supported by the water vapor
PM2.5 17% 27%
SO2 10% 20% conveyor belt.
NOx 46% 46%
VOCs 26% 24% 2. Data and methodology

2.1. Data
pollution emission characteristics in 28 urban locations around Beijing,
Tianjin, Hebei and the surroundings for all types of pollutants decreased
The hourly resolution automatic weather station (AWS) data, surface
during the SF.
and upper-air observation data from National Information Center, China
During the Chinese traditional SF holiday, most urban and rural
Meteorological Administration (CMA), and atmospheric component
areas were experiencing a quasi-negative emissions increment with a
measurements from the Ministry of Ecology and Environment of the
much lower impact of human activities on air quality; the cause of the
People’s Republic of China (PRC) (http://www.zhb.gov.cn/hjzl/) are
heavy foggy haze is therefore, unknown. The following issues are new
used in the study. For further study of the significance of the diagnosis of
focuses of concern stemming from this event.
large-scale and long-lasting aerosol contamination spatiotemporal dis­
The impact of human activities and natural emissions on the climate
tribution, the meteorological conditions PLAM (Parameters Linking Air-
is of particular concern. Research into any potential impact of climate
quality to Meteorological conditions) index is used to discuss the
change processes is very important. In particular, from a global
indicative significance of aerosol pollution spatiotemporal distribution.
perspective, the study of the feedback effects of interactions between
The data for analyzing the heavy pollution in the area around Beijing,
large-scale planetary atmospheric movements and micro-scale atmo­
North China during the SF in February 2020, including condensation
spheric processes on climate change has become an important new focus
rate Fc, wet potential temperature, PLAM index, and super-saturation
(Ge et al., 2012; Graham et al., 2020; Wang et al., 2019a; Zhang et al.,
parameter S, are provided by previous studies (Wang, D.Y. et al.,
2009; Zhang et al., 2012; Zhong et al., 2018a).
2021; Zhang et al., 2009; Zhong et al., 2018b). The other parameters and
First, it has been observed that the Arctic region has transformed
the calculation methods are as follow.
from a sink through pollution snow-removal to a source, which is caused
by melting ice and snow in recent years.
Through a quantitative study of the absorption aerosol optical depth 2.2. Atmospheric low cloud base height
(AAOD) of 550 nm on the surface of Arctic ice and snow absorption
aerosols (BC (black carbon), OC(organic carbon), and dust), Breider The height of the cloud base of a low cloud to obtain the lifting
et al. (2014) discussed the relative contribution of snow-sediment condensation level (LCL) of the atmosphere can be calculated by equa­
removal in transforming the aerosol sink to a source. The study indi­ tion (1) (Wang et al., 2017; Yang et al., 1980):
cated that all of these natural sources are subject to potential feedback ⎛ ⎞
from climate change (Davidson et al., 1989; Kumar et al., 2017; Rahn
es
⎜ 0.622 + 0.622 p− es ⎟
H0 ∈ PLCL ≈ 6.11 × 102 × ⎝ ⎠, (1)
et al., 1977). For example, melting of Arctic sea ice would increase the 0.622 p−eses
source of sea salt and dimethyl sulfide (DMS), and this would act as a
negative climate feedback by increasing both the Arctic AAOD and
where es represents saturated water vapor pressure. In this upper at­
concentration of cloud condensation nuclei (Breider et al., 2014; Xie
mosphere layer, the atmospheric low cloud base height is represented by
et al., 1999). That is, the melting of Arctic ice leads to the accumulation
air pressure (p). When the air pressure (p) of the air mass reaches the
and re-release of aerosols, creating a combined sink–source effect
saturated water vapor pressure (es), but has not yet formed a raindrop, it
(Polissar et al., 2001; Wang et al., 2019a).
indicates a layer of high water content in the atmosphere (Wang et al.,
Second, it is not fully understood if the water vapor transport belt in
2017). Those areas of high atmospheric water content are seen as the
the air, as a sensitive area of aerosol–cloud interactions, contributes to
water vapor flux conveyor belt. The H0 is usually consistent with the
the interaction and synergistic influence on PM2.5 and O3?
actual observed low cloud height (H0); namely, the atmospheric low
Recently, Zhao, Liou, and Gu (Gu et al., 2010, 2011; Zhao et al.,
cloud base height, one of the important parameters for diagnosing the

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J. Wang et al. Atmospheric Environment 272 (2022) 118966

Fig. 2. A diagram of the water vapor flux conveyor belt feature for February 2020 represented by the particular value of water vapor mass calculated by equation (6)
which is refer to the mass passing through a vertical rectangle (δL × δZ) , represented by the shaded area of the rectangle.

weather effects of the water vapor flux conveyor belt. critical value of condensation without raindrops formation, particle
A large-scale high water vapor content area may exist in the atmo­ humidification and new particle acceleration are conducive to forming
sphere locally and the first necessary condition is to have quiet and as secondary aerosol pollution is present in this layer (Kulmala et al.,
stable meteorological conditions in the air mass. That is, an air mass 2004; Shen et al., 2016). This height (H0) is also around the height of the
/
satisfies its attribute as an “iso-θe” process (dθe ≈ 0 ). The wet potential pollution mixing layer (H_PML) (Wang et al., 2017). This may be why
dt
temperature (θe) is given (Yang et al., 1980) as the water vapor flux conveyor belt is both closely related to rainstorms
[( and possibly linked to air pollution.
)Rd ] [( )]
1000 Cp Lws
θe T exp (2)
P CpT 2.3. Atmospheric condensation and super-saturation

Studies indicate that when air-mass properties, such as the wet potential The expression of the condensation function (condensation rate)
temperature (θe), are in a quiet and stable state, as found under an “iso- goes to (Zhang et al., 2005): According to the definition of
θe” process, it is easier to observe a good relationship between the po­ ⎧ /[( )]
tential wet temperature and the high condensation rate (fc), cloud ⎪
⎪ f = f 1 +
L ∂qs
⎪ c cd
structure systematization (H0), precipitation, and the formation of ⎪



Cp ∂T p

foggy-haze in the atmosphere (Browning, 1973; Harrold, 1973; Shapiro ⎪
⎨ [( ) ( )]
and Hastings, 1973). f =
∂qs
+ γd
∂qs (3)

⎪ cd ∂P ∂T p
According to the definition of the wet potential temperature θe in ⎪

⎪ T

equation (2), when the property in a particular layer of atmosphere ⎪

⎩ γ = Rd T

reaches saturation, the saturation mixing ratio W is equal to Ws, and the d
Cp P
initial normalized meteorological condition factor PLAM = I_imc ∝ CθepfTc is
where γd is the dry insulation rate (C◦ m− 1), Cp, L, qs, and fcd are the
reached (Gao and Zhou, 2005; Wang et al., 2012). Because Rd/Cp =
meteorological parameters of specific heat with constant pressure, latent
0.288 is a constant in equation (2), the LCL can be expressed in the air
heat of water vapor condensation, saturation specific humidity, and dry
pressure coordinate system during the iso-θe process.
air condensation rate, respectively. The super-saturation degree is a
Around the height of H0, once the condensation rate fc reaches the
physical quantity that expresses the degree of super-saturation in

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J. Wang et al. Atmospheric Environment 272 (2022) 118966

Fig. 3. (a): the anomaly distribution at 500 hPa average in February 2020 (geo-potential height (H), wind and FH fields. In Fig. 3a, the area corresponding to the
water vapor flux conveyor belt describing by FH > 0.30 × 10− 3×g.cm− 1hPa− 1s− 1 is marked by a red dot line. The height fields (H) is corresponding to the 10-year
average from 2011 to 2020 for February (Unit by the color icon: geo-potential meter × 10). Fig. 3(b): the distributions of monthly average water vapor transport (FH)
at 500 hPa in February 2020 calculating by equation (6)(Unit of the color icon:10− 3×g⋅cm− 1hPa− 1). Fig. 3(c):the average difference distributions (H, T and wind) in
February 2020 corresponding to those in the 500 hPa for February 2019(Unit of the color icon: geo-potential meter × 10), The red lines describe the distributions of
the temperature-differences, “W" is for the high warm center in Fig. 3c.

percentage (Wallace and Hobbs, 2008): meaningful to compare and analyze the influences of weather conditions
in this special period and those in the historical hazy years in Beijing.
S = (e / es − 1) × 100% (4)
The study notes that in the past 10 years since 2010, the average
where e and es are water vapor pressure and saturated water vapor winter and spring weather conditions in North China and surrounding
pressure, respectively. The condensation function (fc) and super- areas have been dominated by haze during the winter monsoon, which is
saturation (S) could form a coordinated and consistent adaptation be­ dominated by the north wind (Wang et al., 2019a).
tween large-scale motion and micro-scale processes of the atmosphere The famous weather proverb is that spring rain is as expensive as oil.
that is both interrelated and constrained. However, in the spring of 2020, the frequent snowfall conditions in
Beijing and northern China were significantly different from the situa­
tions in recent years, especially in the last decade. This indicates that
2.4. Increasing O3 associated with power exponential conversion North China experienced an abnormal atmospheric circulation condi­
tion in the spring of 2020.
With the reduction in NO2 concentration (prior to the 3–6 h for O3), It is generally assumed that after snowy weather there may be more
the O3 concentration increased rapidly with a power exponential con­ clear skies, which facilitates snow removal of pollution under the orig­
version relationship, which indicated that the explosive increasing of O3 inal pollution emissions scenario, and air quality will tend to be good.
meets the NO2-O3 power exponential conversion law (Wang et al., However, Beijing, North China, and other places experienced alternative
2019b). heavy pollution during the snow in February 2020.
To further study the large-scale circulation characteristics of the
O3 = αχ− λ
(5) northern hemisphere in spring 2020 and to compare the differences
between those in recent foggy haze years since 2011, the abnormal
Here, χ is a precursor of O3, NOx, or VOCs, and λ = fc is the condensation
distribution of weather conditions in the northern hemisphere both with
function and α ≈ 10.0 × 103 (Wang et al., 2019b).
latest 10-year’s average and same period in 2019 are given. From a
comparative analysis, a water vapor flux conveyor belt in the northern
3. Results and discussion hemisphere is closely associated with frequent spring snowfalls in Bei­
jing, and has become important.
3.1. Influence of large-scale circulation on the heavy pollution of PM2.5 To discuss the relationship between heavy pollution in Beijing and
and O3 in Beijing and North China North China and the water vapor flux conveyor belt during the SF in
2020, the definition of the water vapor flux conveyor belt is given in this
3.1.1. Water vapor flux conveyor belt and its quantitative identification study first.
This section focuses in particular on what the influence factor is on In Fig. 2, the box superimposed on the background diagram of the
the weather factors for the heavy PM2.5 and O3 pollution observed water vapor flux conveyor belt can indicate the calculation method for
during February 2020 in North China, as well as what the impact is of the upper-level atmosphere calculated by using equation (6). As shown
large-scale circulation currents in the northern hemisphere. It is

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J. Wang et al. Atmospheric Environment 272 (2022) 118966

Fig. 4. a: Hour-by-Hour Distribution of PLAM Index (Red Curve), Atmospheric super-saturation S (Light Blue Bubbles), Distribution of PM2.5 and O3; b: Hour-by-
Hour Distribution of fc (green curve) and atmospheric super-saturation S (light blue bubbles); c: Standardized weather symbols for observing weather phenom­
ena (rain, snow, haze, fog, clear skies, etc.) for February 2020 in Beijing.

in Fig. 2, the water vapor flux conveyor belt refers to the horizontal pressure in northern China was clearly replaced by the warm high
water vapor flux (Fh). In weather analysis and forecasting, the mass of pressure in northeastern China and eastern Mongolia in February 2020.
water vapor transport refers to the flow through the vertical cross- During the SF 2020 in northern China, the warm and high pressure
section in air-pressure coordinates (cm− 1 × hPa− 1) in unit time, which anomaly increased to 120 geo-potential m from the average, replacing
is given as follows (Yang et al., 1980): the cold high pressure center connected to the cold air path from the
⃒ ⃒ polar region (near the Tamil Peninsula) during the haze-heavy years
⃒→⃒
FH = ⃒ V ⃒ q / g (6) (Wang et al., 2019a) (see Fig. 3a and c).
The different weather situations between spring in 2020 and 2019 in
From Fig. 2 we can see a particular value of water vapor mass passing February at 500 hPa are shown in Fig. 3c. In the spring of 2020, the main
through a vertical rectangle (δL × δZ) (represented by the shaded rect­ airflow system, the western Pacific subtropical high-pressure, ranges in
angular area in Fig. 2). Here, δL and δZ are the width and height of the the area from the central Pacific Ocean to the north of 35◦ N. Therefore,
rectangle, respectively. This rectangle needs to be orthogonal to the the location of the subtropical high pressure in the western Pacific is
wind direction (represented by an arrow vector in Fig. 2). The unit is significantly north and west in 2020 compared with 2019. Therefore,
g⋅cm− 1hPa− 1s− 1. In equation (6), g is the acceleration due to gravity, q is under the influence of the easterly wind currents on the south side of the

the specific humidity, and V is the wind speed. In the water vapor flux high pressure in northern and eastern China in the winter and spring of
conveyor belt, V is an important physical quantity, representing the 2020, the thousands of kilometers of strong, warm, humid easterly
momentum supplied for water vapor transport. winds form an important weather system with special effects (see the
It can be seen from Fig. 2 that a high-value water vapor flux (FH) over green arrows in Fig. 3a, b, and 3c).
the upper-level atmosphere is present as a humid/warm eastern-wind As mentioned above, from Fig. 3b, a high-value water vapor flux (FH)
water vapor flux (FH) (high value of FH > 0.3 × 10− 3 g⋅cm− 1hPa− 1s− 1) over the upper-level atmosphere can clearly be seen in the Beijing area,
from the central western Pacific-Ocean (15◦ N, 150◦ E) to the Beijing North China, and the Yangtze River Basin as a humid/warm eastern-
area, North China, and the Yangtze River Basin (marked by the green wind water vapor flux (FH). From Fig. 3a (for air pressure, wind fields,
arrows). and FH fields drawing with the red dotted lines), the green wind vectors
(for the area of high value, FH > 0.3 × 10− 3g⋅cm− 1hPa− 1s− 1) describing
3.1.2. Major differences of weather situations from the usual years the water vapor flux conveyor belt can also be seen clearly. Thus, from
Fig. 3a shows the anomaly average distribution of height and wind Fig. 3a, b, and 3c the green arrows are the same path indicating that the
fields in February 2020 at 500 hPa corresponding to those for the 10- water vapor flux conveyor belt is clearly coincident with the thousands
year average from 2011 to 2020 in February. Fig. 3b shows the distri­ of kilometers of strong, warm and humid easterly winds shown in
butions of monthly average water vapor transport (FH) in February 2020 Fig. 3c.
at 500 hPa calculated by equation (6). Fig. 3c shows the difference in
average distributions (H, T, and wind fields) in February 2020 corre­ 3.2. Influence of micro-scale atmospheric physical process during spring
sponding to those at 500 hPa for February 2019. In Fig. 3a and c, the 2020
anomaly or difference value for the average geo-potential height field is
indicated by the color icon, while the green vector lines describe the 3.2.1. Precursor signals of condensation and super-saturation
streamline differences. The red lines describe the distributions in the Fig. 4a shows the Beijing hourly distribution of the PLAM index and
temperature (Fig. 3c). From Fig. 3a, b, and 3c we can see: atmospheric super-saturation S calculated by equation (4), the obser­
It can be seen from the anomaly distribution of air-pressure in Fig. 3a vations of PM2.5 and O3 in Beijing for February 2020. Fig. 4b shows the
that unlike the same period in more-foggy years, the cold and high distribution of the atmospheric condensation rate fc (green curve),

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J. Wang et al. Atmospheric Environment 272 (2022) 118966

Fig. 5. Daily distribution of the concentration of PM2.5 in Beijing from January to February 2020, and the daily distribution of the Easter wind momentum index(V)
calculated by δH500.

calculated by equation (3). To compare actual weather conditions in humidity, the solution radius is reduced to less than 0.1 μm and the
Beijing hour by hour, Fig. 4c gives a real-time weather report from the super-saturation of S can be increased by more than 12%. The smaller
World Meteorological Organization (WMO) using a weather phenome­ the size of precursors, the smaller the corresponding water droplets
non code and an international standard weather symbol. From Fig. 4, the encountered, the smaller the water process of the micro-particles, which
following can be seen. are not easy to combine by heavy rain droplets (Pruppacher, 1973,;
Wallace and Hobbs, 2008). Studies of Fletcher (1959) showed that
1) The weather conditions described by PLAM index were in a low- super-saturation of 3–10%, could accelerate (within 1 s) the nucleation
value (lower than 20) stage before February 5, 2020. As the PLAM (gas-particle conversion) process in the atmosphere (Fletcher, 1959;
index increased to higher value of >200, the hourly resolution Twomey, 1959).
weather phenomenon of continuing snow and short-term haze were For the above-mentioned 48 consecutive hours of rare snowfall in
observed during the long period from 10:00 on the 5 th to 14:00 on Beijing, the atmospheric super-saturation signal more than 8 d in
the 6 th (see Fig. 4c). advance provided an important microphysical meteorological condition
2) According to Fig. 4c of the hourly resolution of the weather phe­ signal for the contribution of meteorological conditions. Therefore, it is
nomenon digital code report, from 15:00 on February 6 to 14:00 on very important to grasp the impact of the super-saturation atmospheric
February 8 in 2020, after 48 consecutive hours of snow, 42 h of signal S under the condition of the water vapor flux conveyor belt on the
continuous haze was observed (see Fig. 4c). Then the clear sky heavy pollution.
turned during 9:00–20:00 on February 8. At 12:00 on February 11,
values reached 254 μg/m3, and at 12:00 on February 13, they soared 3.2.2. Transport of easterly wind momentum (V) under the water vapor
to 268 μg/m3. It reached the highest value of 268 μg/m3 during the flux conveyor belt
2020 SF holiday. In the water vapor flux conveyor belt, V is an important physical
3) With the PLAM index surge from meteorological pollution condi­ quantity; it is the momentum for water vapor necessary to analyze and
tions, PM2.5 increased cumulatively, while another strong meteoro­ confirm the change characteristics of east wind intensity in the tropo­
logical signal, atmospheric condensation and super-saturation(S) sphere (see Figs. 2 and 5).
signals, were found, which had occurred eight days ahead of the The zonal east wind momentum index can be calculated by the
PM2.5 increment and rose steadily. The condensation rate (fc) gradient of the upper-layer air pressure, where the westerly wind
( )
maintained a high level in the daily variation following obvious rules
strength is described as u = − gf δH z
. The air pressure difference δHz
(peak at 16:00 and trough before 6:00). As early as 00:00 on δn
p
February 1, the condensation rate (fc) reached 1.2 (10− 2 gkg− 1 (the difference of potential height in the isobaric surface, for example
hPa− 1). After ten days, at 16:00 on February 10, fc reached 1.5 (10− 2 δH500) can be a description for the east wind momentum index (Yang
gkg− 1 hPa− 1) (see Fig. 4b, solid line). Correspondingly, super- et al., 1980).
saturation S climbed regularly from 2.5% at 12:00 on the 5th to Fig. 5 shows daily distribution of the PM2.5 concentration in Beijing
2.9% at 23:00 on the 10th and up to 6.1% at 16:00 on the 13th. The from January to February 2020, and the daily distribution of the east
total rising period of S lasted more than 192 h. wind momentum index calculated by the gradient of the air pressure
4) During the highest PM2.5 (268 μg/m3) in Beijing in February 2020, (δH500). From Fig. 5 we can see that:
observations showed that the supersaturated signal S appeared 8 d in
advance. Furthermore, the supersaturated signals S were also 1) The major PM2.5 bursts occurred during January 19 to January 25
continuously shown in advance. It indicated that the super- with from 22 μg/m3 to 261 μg/m3, a total increment of 239 μg/m3.
saturation of the S signal was very important for indicating the The east wind momentum index had increased since 24 h prior, with
pollution anomalies of the 2020 SF. an increment of 23 (see Fig. 5).
2) Additionally, the major PM2.5 bursts occurred from 08:00 February 4
Thus, as mentioned above, on the premise that the emissions of to 08:00 February 13, with the total increment of PM2.5 of 249 μg/
various pollutants decreased overall during the SF 2020, the serious m3. The increment of the east wind momentum index was 17 during
aerosol pollution should have been mainly caused by the influence of the same period (see Fig. 5).
meteorological conditions. 3) The results are consistent with the humid/warm eastern wind water
Studies like Pruppacher (1973) have indicated that at high relative vapor conveyor belt. The important pre-meteorological condition

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J. Wang et al. Atmospheric Environment 272 (2022) 118966

Fig. 6. Hourly distribution of the various weather and atmospheric components during and after the foggy-haze period on 12th-17th February. The blue solid line
and dot line are the observations of PM2.5 and its fitted curve; The green solid line and the dot line are the (O3 6 h ago) δNO2 and its hourly change fitting curve. The
red solid line and the dot line are ξ = δO3 and its hourly change fit curve based on the power exponential conversion law, the conversion from NO2 to O3 calculating
by equation (5) in section 2.4.

signal for aerosol pollution, super-saturation S, is an important δNO2 dropped from 19:00 on the 12 th at 121 μg/m3 to − 47 μg/m3 at
feature of the east wind momentum transport due to the water vapor 06:00 on the 17th (see Fig. 6a, green solid line).
flux conveyor belt. Notably, O3 was in contrast to the downward trend of NO2. From the
fitted curve of the hourly change of δO3 based on the power exponential,
3.3. p.m.2.5 and O3 superposition-composite pollution event it can see that an upward trend of δO3 was given. The correlation
confirmation coefficient (R2) of the fit curve reached 0.68, and the
3.3.1. Observation facts of conversion from NO2 to O3 under the condition correlation significance level exceeded 0.001 (see Fig. 6a, red dotted
of high condensation line). The growth peaks of O3 were observed up to 131 μg/m3, on 13th
Fig. 6 shows hourly distribution of the various weather and atmo­ February (see Fig. 4). This type of O3 growth processes occurred
spheric components during and after the fog-haze period on February frequently in February.
12–17, including the PM2.5 observations and its fitted curve; the δNO2 As can be seen from the 3 annotation boxes in Fig. 4, three significant
observations and its hourly change fit curve, as well as the O3 increment growth peaks of O3 were observed, 131, 79, and 90 μg/m3, respectively,
(δO3) of conversion of NO2 to O3 calculated by equation (5) based on the which appeared on February 13, 21, and 29, respectively. Before the
power exponential conversion law, and its hourly change fit curve. Ac­ peak of O3 appears, it corresponds to the previous period of atmospheric
cording to Fig. 6, on February 12–14, the PM2.5 observation continued to humidity, including the process of gradually increasing supersaturation
soar, reaching 268 μg/m3 at 12:00 on the 13th. However, during the to 6.1%, 4.2% and 4.9%, respectively (shown in the dotted vector in
period from February 14–17, the PM2.5 observation and its hourly rate of Fig. 4). Its early start date can be traced to the 11th, 19th and 28th, 24
change fitted curve showed an e− exponential downward trend. The ~72 h earlier, respectively. In Fig. 6, according to the power function
confirmation coefficient (R2) for the fitted curve was 0.75, and at 08:00 equation (5)(which describing the physical mechanism tha NO2
on the 15th, the PM2.5 observation dropped below 20 μg/m3 (see Fig. 6a, decreasing in the previous few hours and then increasing O3 based on it),
blue solid line). Meanwhile, during February 12–17, the δNO2 obser­ the increment of O3 (δO3) has an opposite synergistic trend with the first
vation and hourly change fit curve also showed a nonlinear downward 6 h of NO2, that is, NO2 decrease occurs first, the O3 increment (δO3) is
trend. The confirmation coefficient (R2) of the fitted curve was 0.70, quasi-synchronously sustained, but period of increment (δO3) occurs in

Fig. 7. a the correlation analyses between hourly O3 and 6 h prior NO2 measurements, Fig. 7b the diurnal cycle synthetic sections of O3, 6 h prior δNO2 concen­
trations and the changes of height of low cloud (δH0), Fig. 7c the correlation between PM2.5 as well as O3 and H0 in February 1 to 29, 2020 in Beijing.

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J. Wang et al. Atmospheric Environment 272 (2022) 118966

Fig. 8. a: The hourly evolution of height of


low cloud during 7–12 February 2020, b:
The hourly evolution of O3 during 7–12
February 2020,c: The hourly evolution of
PM2.5 during 8–13 February 2020,d: The
hourly evolution of height of low cloud
during 12–17 February 2020,e: The hourly
evolution of O3 during 12–17 February
2020,f: The hourly evolution of PM2.5 dur­
ing 16–21 February 2020, g: The hourly
evolution of height of low cloud during
23–28 February 2020, h: The hourly evolu­
tion of O3 during 23–28 February 2020,i:
The hourly evolution of PM2.5 during
24–29February 2020.

cumulative lag. They are significantly correlated. This suggests that in a Thus, the quasi-synchronous characteristics of the O3 growth corre­
high humidity (high condensation rate Fc) environment, the NO2 sponds to the NO2 decline that the explosive increasing of O3 meets the
described in the power function equation (5) decreases first, and the O3 NO2-O3 power exponential conversion law (ξ = αχ− λ)driving by the at­
lags in growth, which results in additional increments of O3 in the mospheric condensation and humidification process under the high
impact of meteorological conditions. humidity condition (namely high precursor signals of condensation and

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J. Wang et al. Atmospheric Environment 272 (2022) 118966

super-saturation) of the water vapor conveyor belt (Niu et al., 2020; July 2008 in Beijing, H0 was positively correlated with the concentration
Wang et al., 2019b). of O3 but negatively correlated with PM2.5. A decrease in H0 created a
favorable condition for the accumulation of PM2.5, and an increase in H0
3.3.2. Superposition-composite effects of PM2.5 and O3 due to daily cycle led to O3 concentration increasing. Given that O3 falls into the secondary
changes of H0 pollution category, all pollutants are feedback and accumulate in the
Fig. 7a shows the correlation analyses between hourly O3 and the 6-h atmosphere, thereby causing the overlaps of one pollutant with another
prior NO2 measurements for February 1–29, 2020 in Beijing. Fig. 7b and eventually aggravating the pollution (Wang et al., 2019b; Zhang
shows diurnal cycle synthetic sections of O3 and the 6-h prior δNO2 et al., 2009). The study indicated that the H0 rise at daytime and H0
concentrations as well as the changes in height of low clouds (δH0). decrease at night is closely related to the daily cycle of the sun’s zenith
Fig. 7c shows the correlation analyses between PM2.5 as well as O3 and angle. This result is an important observational fact and therefore de­
H0 during February 1–29, 2020 in Beijing. serves adequate attention (Wang et al., 2019b). As mentioned above,
From Fig. 7a, it can be seen that a significant negative correlation of those daily changes in the microphysical meteorological processes of
the power exponent for the hourly O3 with the 6 h prior NO2 measure­ atmospheric cloud characteristics may form the interactive super­
ments is observed. The correlation determination coefficient (R2) was position influence effects on the PM2.5 and O3. Those types of observa­
0.15 with the correlation significance level exceeding 0.001. Thus, the tional facts are further seen in Fig. 4a. A surge in both of PM2.5 and O3
increase in O3 was closely related to the decrease in nitrogen oxide Nox concentrations occurred, 268 μg/m3 and 131 μg/m3 respectively on
3–6 h prior. February 13. Therefore, to learn what the mechanism is, here we discuss
Fig. 7b shows a composite profile of the daily hourly distribution the situation during February 7–13, 2020 in more detail.
cycle in Beijing in February 2020. We can see from Fig. 7b that NO2 Fig. 8a, b, and c show the hourly evolution of low cloud height (H0),
decreased from early morning to daytime. The value of NO2 decreased O3, and PM2.5 during February 7–12, 2020, respectively (Fig. 8c refers
by up to 50 μg/m3 (blue double arrow in the lower left corner of the to February 8–13, 2020). The description and the format in Fig. 8d, e and
figure) during the 6-h period before sunrise (δh = 6 h). From 07:00 to 8f are the same as in Fig. 8a, b, and c, but the period is for February
14:00, the low cloud height (H0) rose to 800 m (the time period is 12–17, 2020. Fig. 8f refers to February 16–21, 2020. The description and
indicated by the green double arrow in the figure). Merely 10 h later (at the format in Fig. 8g and h and 8i are the same as in Fig. 8a, b, and c, but
16:00), the O3 concentration jumped to 110 μg/m3 (see the red double the period is for February 23–28, 2020. Fig. 8i refers to February 24–29,
arrows). This result indicated that a prior decrease in NO2 concentration 2020. The following observations can be seen from Fig. 8.
was followed by the rising of O3 concentration after sunrise, which was The hourly evolution of low cloud height (H0) indicated that daily
an ongoing microphysical process. variation in low cloud heights calculated by equation (1) were clearly
The results show that after sunrise, with the rise in low cloud height, visible. The rise in H0 in the daytime and the decrease in H0 at night
NO2 concentrations decreased first, and then O3 concentrations rose in a were observed during February 7–12, 2020 (see Fig. 8a), February
continuous atmospheric physical micro-scale process associated with 12–17, 2020 (Fig. 8d) and February 23–28 (Figs. 8g), 2020. Consistent
the solar zenith angle. with the daily changes in low cloud heights, (i.e., the conversion
Taken together, as mentioned above, in Fig. 7b, the cumulative su­ increment δO3 from NO2 to O3) driven by fc, also changed consistently.
perposition analysis of each day is performed hour by hour in February, The rise in daytime δO3 and the decrease in δO3 at night were observed
and the contribution of the previous decay of NO2 to the growth of O3 is during February 7–12 (see Fig. 8b).
described by comparing the correlation between the “6 h prior δNO2 As mentioned above, the concentration of PM2.5 increases with the
concentrations” change and the growth of O3. That is, an attempt was decrease of H0 at night, and PM2.5 will gradually accumulate with the
made to observe the observational fact that the pre-decay of NO2 was increase of H0 during the day, which respectively referring to two types
associated with the presence of an increase in ozone concentration at of mechanisms. That is, the double superposition mechanism. Due to the
least 6 h later, including in the afternoon. decrease of H0 at night, the concentration of the original existing PM2.5
As can be seen from Fig. 7b, in the larger data of hourly resolution, is increased due to unfavorable diffusion; With the rise of H0 during the
the proportion of positive values of δNO2 is lower than 1/3 to 1/4. The day after a few hours, it will cause secondary aerosol pollution of new
absolutely dominant for the negative δNO2 values appeared from 6:00 to particles due to emissions, resulting in the accumulation and increase of
8:00 in the morning, which was in the period 6 h before the peak of O3, PM2.5 concentration.
namely for he period at 12:00–17:00 in the afternoon. In particular, the It is seen from Fig. 8 that the observations of comparative examples,
trough of δNO2 value occurs at 6 to 9 o’clock in the morning, and the including the three pollution periods observed in February 2021 indi­
peak of O3 occurs at 12 to 17 o’clock in the afternoon. It shows that cated that the increase in ozone concentrations in February can form a
meteorological conditions have an additional contribution to the partial “increment” of O3. Coupled with the increased meteorological
reduction of NO2 in the early stage and the appreciation of O3 in the later conditions of the concentration of secondary pollutants during the day.
period. That is, the interaction between meteorological conditions and emis­
Fig. 7c shows the correlation between PM2.5 as well as O3 and H0 in sions to form a compound pollution.
February 1 to 29, 2020 in Beijing. PM2.5 and O3 are related to the power It is seen also from Fig. 8 that After 14:00 on February 7 (for local
index of negative and positive, respectively, with and low cloud height, time, the same as in below), that is, the sun Zenith angle when the top
and the correlation confirmation coefficient (R2) is 0.3 and 0.2, (illustrated“ ”), O3 peaked up to 60 μg/m3, the peak increased daily
respectively. The correlation significance level exceeds 0.001. Thus it (see Fig. 8b). After a continuous daily accumulation, the accumulation
can be seen, daily changes in the microphysical meteorological pro­ peak of PM2.5 was up to 200 μg/m3 at 14:00 (when the sun’s zenith angle
cesses of atmospheric cloud characteristics can form the interactive su­ was at the moment of “the top”) on February 9, and then stable to high
perposition influence effects on the PM2.5 and O3. These observations value of 240 μg/m3. A lag in the accumulation of PM2.5 peaks has been
are further confirmed in Fig. 4a. A surge in both of PM2.5 and O3 con­ observed also in two other cases in February (16–21 (Figs. 8f) and 24–29
centrations occurred, 268 μg/m3 and 131 μg/m3, respectively, on (Fig. 8i)). Therefore, based on the results given in this study, the su­
February 13. perposition composite mechanisms of O3 and PM2.5 pollution can be
clearly observed by the interaction of large-scale water vapor transport
3.3.3. Mechanisms of superposition composite pollution for O3 and PM2.5 with microphysical meteorological conditions.
The study of the correlation between hourly observations of PM2.5,
O3, and H0 show that during the heavy pollution in September to
December 2005 and 2016 in Beijing, Hangzhou and Chengdu, as well as

9
J. Wang et al. Atmospheric Environment 272 (2022) 118966

Fig. 9. The physical concept illustration of the special pollution process in Beijing during the Spring Festival 2020 that the interaction between large-scale water
vapor transportation and microphysical meteorological conditions provides a significant contribution to the formation of O3 and PM2.5 superposition-
composite pollution.

4. Conclusions This is an important mechanism of meteorological condition impacts


on composite pollution of O3 and PM2.5.
The findings in the study are as follows.
Declaration of competing interest
1) Unlike the weather conditions with more haze in previous years, the
heavy pollution event during the spring 2020 snow in Beijing is
The authors declare that they have no known competing financial
associated with the water vapor conveyor belt in the northern
interests or personal relationships that could have appeared to influence
hemisphere, which is an important support for the formation of
the work reported in this paper.
heavy haze pollution during snow in Beijing and the surroundings,
rather than snow removal purifying the atmosphere. This study re­
Acknowledgments
veals that the interaction between large-scale water vapor trans­
portation and microphysical meteorological conditions provides a
The authors would like to thank Academician Zhang X.Y. for his
significant contribution to the formation of O3 and PM2.5
valuable suggestions and comments. This study is supported jointly by
superposition-composite pollution.
NSFC Major Project (42090030), the NSFC Project (U19A2044); the
2) The interaction of large-scale water vapor transport and weather-
National Key Project of MOST (2016YFC0203306), National Natural
scale processes is shown as the rise in low cloud height (H0) at
Science Foundation of China (41675121), the Basic Scientific Research
daytime and the decrease in H0 at night. The ascent in H0 led to O3
Progress of the Chinese Academy of Meteorological Sciences
rising. Given that O3 is considered secondary pollution, following the
(2016Z001), the National Key Project of Basic Research
cycle of daily periodic changes in cloud height (H0) (see the 3 block
(2014CB441201, 453172).
diagrams to the right of Fig. 9), the decrease in PM2.5 at night is offset
partly by an increment in concentrations of secondary pollutants
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