Overall regional pollution situation of in Guangxi. From 18 to 24 February, 2020, a regional air pollution event with a cumulative pollution period of 1.1 days occurred in Guangxi, and the key pollutant was PM2.5 (see Supplementary Fig. S1). During this period, this pollution event first started on 19 February, and slight pollution (AQI >100, PM2.5> 75μg.m−3) was identified in four cities, namely Laibin, Chongzuo, Liuzhou and Hechi; among of them, Chongzuo represented the highest AQI value (AQI=123). However, the most severe pollution was observed in Hechi city on 20th Feb (AQI> 200, PM2.5>150 μg.m−3), then the levels of pollutants began to decline (with slightly rise up on 23rd of February) and finally ended on February 24.
To evaluate the regional overall pollution status of Guangxi during this period, the comparison of average concentrations of atmospheric PM2.5 in Guangxi during 19-23 Feb 2020 with those of all other provinces was illustrated in Supplementary Fig. S2. It showed that the average PM2.5 concentration was 61 μg.m−3, which was the third highest for nationwide in these days (the average PM2.5 concentrations in Hechi city even reached up to 79 μg.m−3). In contrast, the average atmospheric PM2.5 concentrations in surrounding provinces, e.g., Guangdong, Yunnan, Guizhou and Hunan were only 31, 35, 44 and 46 μg.m−3 respectively, which were significantly lower than that of Guangxi. This indicated that the pollutants could potentially originate from local sources rather than the transmissions from the neighboring provinces. Interestingly, although the influence of industrial and domestic activities had been reduced to a minimum extent within Guangxi or neighboring provinces during the COVID-19 lockdown, the regional pollution event in Guangxi did take places. Accordingly, we carried out the cause analysis of this PM2.5 pollution event based on the data from different kinds of equipment installed in Scientific Research Academy of Guangxi Environmental Protection.
The data representativeness in the sampling site. In order to evaluate the representativeness of the data measured in the sampling site, the homochronous data released by the national real-time municipal air quality platform (http:// 106. 37. 208. 233: 20035) of China National Environmental Monitoring Centre (CNEMC) were employed for the comparison (see Supplementary Table S1). It showed that the daily average values of PM2.5, PM10, SO2, NO2, O3 and CO were relatively consistent within these two monitoring systems. The correlation analysis of hourly data of PM2.5 and CO showed in Supplementary Fig. S3. The correlation coefficient for the two pollutants were both above 0.93, which indicated an excellent representativeness of data was recorded in the station for the ambient air quality of SRAGEP in reference to CNEMC.
Overall air pollution situationin Nanning City.
The time series of mass concentration of atmospheric pollutants along with key meterological conditions in Nanning city from 18 to 24, Feb 2020 were illustrated in Figure 1. According to the PM2.5 concentration variations, the whole progression of pollution could be divided into three stages, i.e. pre-pollution period (PPP), pollution accumulation period (PAP) and pollution dissipation period (PDP). The corresponding average PM2.5 concentrations for PPP, PAP and PDP were 32, 73, 35 μg.m−3, respectively, PM2.5 concentration of PAP was twice as high as those of the other two stages. Similarly, the average concentrations of CO in PAP (1.00 mg/m3) was also higher than those of PPP and PDP (0.57 and 0.90 mg.m-3, respectively). Interestingly, while PAP and PDP possessed the average relative humidity (RH) 71% and 70%, respectively, the average of RH in PPP was only 36%. The main reason could be the lower wind speed (WS) in PAP (0.71m/s) than those of PPP (0.87 m.s-1) and PDP (1.19 m.s-1). Additionally, the average planetary boundary layer heights (PBLH) were 1253 m, 787 m and 987 m in PPP, PAP and PDP, respectively. Moderate atmospheric pollution was identified in Nanning city on 20 Feb with a PBLH ranged from 297-934 m on that day. Generally, PBLH is higher during the daytime, especially at noon, however, a minimum value of PBLH (297m) was observed at 11 a.m. on 20 February, which indicated that the potential adverse meteorological conditions for the horizontal and vertical diffusions of pollutants could result in the high PM2.5 concentration on that day. However, during PDP, particularly on 24 Feb, the atmospheric diffusion conditions were in favor due to the low air pressure near ground and airflow currents towards the south direction, thus the calm weather maintained for several days was mitigated through the enhanced airflow conditions, as a result, the air quality began to be improved.
Single particle source analysis. By analyzing the composition of particulate matters, the sources of PM2.5 in municipal area could be categorized into: catering (kitchens), dust, biomass burning (BB), vehicle exhaust, coal, industrial process (non-combustion process), secondary inorganic source and others (Figure 2). It showed that the dominant source of PM2.5 in the stage of PPP was BB (accounts for 40.4%), followed by secondary inorganics (accounts for 28.1%) and motor vehicle exhaust (11.7%). In contrast, secondary inorganics dominated in PAP (56.1%) and PDP (30.2%), and it seemed that there was an obvious increasing of secondary transformed particulates during the PAP. The second largest contribution sources of PM2.5 in PAP and PDP was BB, which accounts for the proportions of 17.4% and 26.1%, respectively. By analyzing the fire spots map of satellite remote sensing monitoring, large numbers of fire spots were identified in Nanning city and regions around, however, there was no significant pollution generated attributed to relatively better meteorological diffusion conditions on February 18-19. As the atmospheric horizontal and vertical diffusion conditions were worsened afterwards, pollutants began to accumulate and produce more particulates of secondary transformation, which induced more severe PM2.5 pollution on February 20.
As mentioned above, BB had been confirmed to be the largest contribution to the pollution source during the PPP and the second largest contributor in the other two stages. Fire spots maps were constructed based on data of satellite remote sensing (Figure 3), the straw incineration fire spots were identified from February 18 to 24. The total count of straw fire spots in Guangxi was 421, and 52 of them were in Nanning city, while 70, 45 and 44 fire spots were distributed in three cities border on Nanning (Laibin, Chongzuo and Guigang, respectively). The fire spots of these four cities were the most intensified among 14 cities of Guangxi during the period of observation, which implied that the pollution in Nanning was attributed to the regional BB. As the three largest sugar production cities of Guangxi, Nanning (No.1), Laibin (No.2) and Congzuo (No.3) possess large areas of sugarcane farming that produces large amount of waste sugarcane leaves. The open-air incineration of sugarcane leaves induces significant difficulties in regional air pollution reduction particularly the urban atmospheric pollution control. It has been reported that the incineration of agricultural straw posed significant effects on air quality, public health and climate in China17-19. In northern China, pollution due to the straw incinerations usually take place in autumn20, for instance, the open BB contributed 52.7% of atmospheric PM2.5 in Northeast region of China during November 1-4, 2015. However, there is little research on how BB affects air quality in Southern China. Guangxi has the highest pollutants emission from BB among 31 provinces in China21. During the new-corona epidemic control period, pollution from other sources such as industry, automobile vehicles were significantly decreased, however, the activities of straw incinerations in vast rural regions kept going on as per traditional farming seasons. The observation of NO2 concentration increased at about 12:00 and reached the peak at about 18:00 which was consistent with the practice of farmer usually burning the straw in afternoons.
Statistics of aerosol light absorption coefficient and AAE. Mean values of aerosol light absorption coefficients σabs at seven wavelengths and AAE during different stages are summarized in Table 1. During the COVID-19 strict control period, the light absorptions of both ultraviolet (σabs,370) and infrared (σabs,880) wavelength in Nanning were significantly lower than reported data that in Xiamen22 and in Lhasa23.
Stages
|
σabs,370
(Mm-1)
|
σabs,470
(Mm-1)
|
σabs,520
(Mm-1)
|
σabs,590
(Mm-1)
|
σabs,660
(Mm-1)
|
σabs,880
(Mm-1)
|
σabs,950
(Mm-1)
|
AAE
|
PPP
|
23.5
|
12.5
|
9.6
|
7.6
|
6.3
|
3.5
|
3.0
|
2.2
|
PAP
|
15.3
|
8.9
|
7.0
|
5.7
|
4.7
|
2.7
|
2.3
|
2.0
|
PDP
|
3.8
|
2.5
|
2.0
|
1.7
|
1.4
|
0.8
|
0.7
|
1.7
|
Table 1. Aerosol light absorption properties.
It should be noted that the value of AAE could be used as an indicator of aerosol from burning processes of fossil fuel or biomass24, as the major content of fossil fuel burning is black carbon (BC), thus, the AAE of aerosol caused by fossil fuel burning is close to 125,26. In contrast, aerosol from BB contain rich amount of brown carbon (BrC), so it could generate even larger AAE than that from fossil fuel24. In this case, AAE value of aerosol from BB was usually larger than 2.027. In this study, AAEs of PPP and PAP were 2.2 and 2.0 respectively, which implied that aerosol absorptions in Nanning city could be influenced by the burning of both biomass and fossil fuel. Additionally, considering the significant reduction of fossil fuel consumption during the special control period of new-corona epidemics, the BB could be the dominator factor resulting in the higher AAE in PPP and PAP, which was also supported by the large number of fire spots detected by satellites (commercial data) ( Figure 3).
Impact analysis of secondary pollution.The formation of secondary particulate matter might also significantly contribute to this pollution event, this conclusion was based on the following two reasons. The first is the synergistic effects of NO2, NH3 in the condition of high relative humidity on promoting the liquid-phase oxidation of SO2, which leaded to the obvious increase of sulfate particulates in PAP. Figure 4 shows the relationships between sulfate particle number concentration with levels of SO2, NO2, NH3 and RH, and it seems that the positive correlations between concentration of sulfate particulates and NO2, NH3, RH were identified during the PAP with relatively better linearity. However, in the stage of NPAP (PPP and PDP), there was no significant linearity correlation even between SO2 with sulfate particulate identified. During the whole observation period, the concentration of SO2 remained at a relatively stable level maybe due to the reduction of industrial emission and absence of obvious SO2 source around the observation site in the central district of Nanning city, and there was no significantly increase of SO2 concentration even during the stage of PAP when the height of boundary layer decreased. Interestingly, the concentrations of sulfate particulates showed the positive correlation relationships with NO2, NH3 and RH during PAP. It may be caused by the coexistence of NO2 and NH3 could promote the conversion of SO2 to sulfate particulates under the condition of relatively high humidity, which has been reported in the previous studies through both experimental simulation and on-field observations and NO2 would enhance the liquid phase oxidation of SO2 in the cloud process or in the existence of NH3 under high RH conditions. Additionally, Wang et al.28adopted the method of Density Function Theory (DFT) to investigate how H2O and NH3 promoted the oxidation reaction of SO2 and NO2, and found that NH3 played an important role in stabilizing the complex products. Chen et al.29employed the glassware reactors and demonstrated that NH3 could increase the dissolution of SO2 and hence enhanced the liquid-phase oxidation of SO2.
Secondly, the increase of secondary particulates could be explained by the positive feedback mechanism of pollution boundary layer (PBL)-relative humidity (RH)- secondary particles matter (SPM)-particulate matter (PM), which has been proposed in the previous studies, and the relative humidity (RH) and the PBLH are essential factors which may affect the formation of atmospheric PM2.5 30,31. The positive feedback mechanism of PBL-RH-SPM-PM suggests that PM level and RH would be low while PBLH is high at the beginning stage of a haze event. Since the atmospheric diffusion condition could be adversely changed by weather situation, PM would begin to accumulate, then the radiation effects due to the increase of PM could cause PBLH decreasing, and further induce the increase of PM and RH. On the other hand, the moisture absorbed by PM would increase and enhance the radiation effect which could further decrease PBLH. Thus, RH would keep increasing and accordingly enhance the formation of SPM. So, through the comprehensive analysis of extinction coefficient, PBLH, PM and RH which were observed by lidar, it is concluded that PBL-RH-SPM-PM positive feedback mechanism is an ideal model to elucidate the occurrence and development of the pollution.
Figure 5(a) and (b) show the time series of the vertical distribution of the extinction coefficient and depolarization ratio of the lidar at 532 nm from February 18-24, 2020, respectively. They demonstrate that the near-ground extinction coefficients for Nanning were relatively small in PPP and gradually increased; its depolarization ratio was relatively small with little variation for the whole observation period. The PBLH gradually reduced from about 2 km to 1 km which was adverse for atmospheric convection and resulted in the atmospheric diffraction condition worse, thus the pollutants began to accumulate as concentrations of PM2.5 and secondary inorganics aerosol (SIA) levels slowly increased (Figure 5(c) and (d)). Specially, at 12:00 on February 20 in PAP, the wind speed was small and PLH was relatively low (minimum values was 293 m only), the atmospheric diffusion condition turned even worse and accordingly caused the cumulative accumulations of pollutants. At about 0:00 20 Feb, the extinction coefficients near-ground suddenly increased, meanwhile, the concentration of PM2.5 and SIA level also rapidly increased and reached peak value (179 ug.m-3 for PM2.5). From 00:00, Feb. 20th to 12:00, Feb. 21st, the boundary layer was slightly uplifted, and the wind speed got faster, then the vertical diffusion conditions improved and the level of pollutant consequently declined. Afterwards, the boundary layer dropped and wind speed decreased from 12:00 to 22:00 on Feb. 21st, and PM2.5 and SIA level continued to rise to reach the peak. From 0:00 to 21:00 on Feb. 22nd, the diffusion capability was relatively good, PM2.5 and SIA decreased gradually, however, at 22:00, near-ground distinction coefficient suddenly increased, PM2.5 and SIA rose up and reached a peak value again at 0:00 23rd. Then PM2.5 and SIA gradually decreased with atmospheric diffusion, and at 0:00 23rd, extinction coefficient rose up again, PM2.5 and SIA climbed up slowly afterwards. Finally, in the period of PDP, boundary layer was uplifted, wind speed got stronger, the overall atmospheric diffusion condition turned better with relatively small amount of pollutant emissions near ground, thus the levels of PM2.5 and SIA stepwisely declined and maintained at relatively low levels.
It could be concluded that near-ground PM2.5 accumulated as PBLH significantly decreased, other factors including the increase of moisture level, higher RH and local straw burning also resulted in the slight pollution. Additionally, the extinction coefficient would increase with the increase of PM2.5; PBLH would be further lowered down, and with the increase of RH, more moisture would be absorbed by PM2.5, which could enhance the gas-particulate formation to generate more SIA. In all, the high RH, low PBLH, poor horizontal and vertical atmospheric diffusion capacities combined with the effects of local straw burning, made the pollution gradually turn worse. Thus, on February 24, PBLH was obviously uplifted, and wind speed got faster, then the diffusion factors turned better, and then the air quality improved.
Analysis for the pollutions from regional transportation. It is well known that pollutants generated by BB could be transported to long distances32,33. As there were many fire spots identified in the regions around Nanning City, the pollutions from regional transportation should also be considered. The HYSPLIT model proposed by NOAA (https://www.arl.noaa.gov/) was adopted to analyze the airflow back trajectory of pollutants during the sampling period. Airflows at the heights of 500 m, 1000 m and 2000 m were selected to calculate the backward trajectory figure (Figure 6(a), (b), (c), (d)). From February 18 to 21, the air masses of 500 m and 1000 m were mainly influenced by the air flows from Guangdong Province and Beibu Gulf located in the southeast direction, while air masses at 2000 m were mainly influenced by the airflow from Vietnam. Based on the satellite remote sensing monitoring maps (Figure 6.), it was found that lots of fire spots were in Vietnam, Laos, Thailand and Cambodia during the period of pollution event occurred in Nanning. The backward trajectory calculations indicated that the long distance transportation of biomass incineration pollutants from these countries would have some influence on the regional atmosphere in Nanning. Recently, Yue et al.34 showed that CO level near the ground decreased 17% compared with the same period of the previous year, while the concentration of CO in troposphere increased by 2.5%. These also supported the previous conclusion that long distance transportation of biomass incinerations from foreign countries could affect the atmosphere in the south of China. In this study, the increase of CO level during PAP in Nanning was identified, and it was also believed due to the influence of BB both in reginal cities and in Southeast Asia. Interestingly, on February 22 (Figure 6(e)), it had been showed that the origins of air masses at 500m, 1000m and 1500m were from localities within Nanning. Based on the analysis of meteorological land weather conditions, it was found that the pollutants accumulated as a wind convergence zone was over Nanning that day. However, on February 23 (Figure 6(f)), the airflow was from cities including Laibin and Guigang which had the relatively intensive fire spots; on February 24 (Figure 6(g)), the airflows of three heights were mainly from neighboring Guangdong province and Beibu Gulf, and as the meteorological diffusion conditions had been improved, thus the pollution began to gradually dissipate. Overall, based on the analysis of fire spots contribution maps and backward trajectory, it had concluded that the air masses had passed the regions of intensive fire spots, and this PM2.5 pollution event in Nanning was generated not only from local BB but also from transportation from surrounding countries in Southeast Asia.