3.1 Characteristics of PM10 and PM2.5
Daily concentraiton’s fluctuation of PM10 and PM2.5 in Hefei City is shown in Fig. 2. From 2018 to 2020 the annual averaged concentrations of PM10 and PM2.5 were 66.74 ± 33.05 µg·m− 3 and 38.08 ± 23.05 µg·m− 3, respectively. Of three years, PM10 (58.84 ± 28.67 µg·m− 3) and PM2.5 (32.05 ± 18.64 µg·m− 3) had the lowest concentrations in 2020 (p > 0.05). Also, the levels of PM in 2020 were either lower than or similar to the criterion as 70 µg·m− 3 for PM10 and 35 µg·m− 3 for PM2.5 required by the Class II standard of the Chinese Ambient Air Quality Standards (GB 3095 − 2012). This means that the air quality of Hefei city has been improved considerably recently. However, the concentraion of PM10 was still higher than the annual average concentrations of 64 µg·m− 3 of 168 Chinese cities in 2020 [11]. As to the ratio of PM2.5 to PM10, it did not fluctuate significantly over the study period with averages of 0.60 ± 0.71 in 2018, 0.56 ± 0.18 in 2019 and 0.57 ± 0.19 in 2020. The value of PM2.5/PM10 were lower than those, calculated with the data from [11], of Beijing (0.67), shanghai (0.78) and Tianjin (0.71), while similar to that of Nanjing (0.55) and Guangzhou (0.53).
[Fig. 2 Daily variation of particulate matter in Hefei city between 2018 and 2020]
As shown in Fig. 3 (a), between 2018 and 2020 the averaged concentrations of PM in spring, summer, autumn and winter were 73.41 ± 30.04, 45.80 ± 16.50, 72.75 ± 35.10 and 81.81 ± 38.17 µg·m− 3 for PM10 while 38.73 ± 15.73, 24.26 ± 10.73, 37.16 ± 19.60 and 61.42 ± 32.16 µg·m− 3 for PM2.5. PM10 and PM2.5 had the same seasonal concentration variation, the highest in winter while the lowest in summer. Meanwhile, the pollution level of PM10 and PM2.5 in spring was nearly the same to that of autumn (p < 0.001).
Person correlationship analysis suggests that in Hefei city PM2.5 was significantly related with PM10 (p < 0.001) with correlation coefficient (r) as 0.557 in spring, 0.822 in summer, 0.688 in autumn and 0.899 in winter. Based on the record by Shen [21] on Hefei, the values of r in spring, summer, autumn and winter during 2015–2017 were 0.811, 0.913, 0.925 and 0.947, respectively. It means that the relationship between PM10 and PM2.5 had been weakened by a small margin. Therefore, the pollution sources contributing PM10 and PM2.5 also had changed correspondingly. On the other hand, the values of PM2.5/PM10 were roughly the equivalent during spring (0.56 ± 0.19), summer (0.53 ± 0.14) and autumn (0.53 ± 0.17) (p > 0.05). And the winter had the highest ratio as 0.75 ± 0.16. This indicates that the atmospheric pollution type of Hefei by PM in winter was different from other seasons.
[Fig. 3 Seasonal variation of particulate matter in Hefei city between 2018 and 2020]
[Fig. 4 Correlationship between PM10 and PM2.5 with respect to season n Hefei city between 2018 and 2020]
3.2 Trajectories cluster
Trajectories were categorized into six clusters by the present study for each season (Fig. 5). And the analysis on PM corresponding to six clusters is summarized in Fig. 6 and Table 1. The pathways of air flow in summer were different from that of other seasons. The trajectories mainly came from the southern inland and the East China Sea during summer while from the north China and the northwest China in spring, autumn and winter. Comparatively, the migration pathway of air mass was the shortest in summer. Shi et al. [22] identified the seasonal trajectories reaching Hefei city during 2001 ~ 2005 and found they were mainly sourced from the northwest of Hefei city during spring, summer and winter, which was in accordance with the present study. However, the migration pathway got short during 2018–2020 regardless of season. Also, the air mass originated from Mongolia became rare.
[Fig. 5 Clusters of back trajectories of air flow for Hefei City between 2018 and 2020]
[Fig. 6 PM10 and PM2.5 portioned by trajectory cluster of air flow for Hefei City between 2018 and 2020]
The air mass of trajectories in spring accounted for 15.22%, 19.72%, 23.83%, 3.72%, 18.84% and 8.67% for cluster 1 to 6, respectively. Cluster 1 (northwest→southwest) had the highest PM10 as 93.37 ± 39.22 µg·m− 3, followed by cluster 4 (northwest) as 89.29 ± 44.17 µg·m− 3 and cluster 3 (northwest→south) as 81.04 ± 41.80 µg·m− 3. Also, cluster 1 was coupled with the highest PM2.5 of 44.09 ± 19.11 µg·m− 3. The levels of PM2.5 from cluster 3 and 4 were almost the same, which was slightly smaller than that of cluster 1. In spring PM10 and PM2.5 in Hefei were averaged at 73.41 and 38.73 µg·m− 3, respectively. Concentrations of PM10 at cluster 1, 3 and 4 were higher than the average concentration of winter in Hefei, while PM2.5 at cluster 1 to 5. Therefore, air mass from cluster 1, 3 and 4 is considered as the major transport pathway that PM migrating to Hefei in spring. The air mass of cluster 1 started from Fen-wei Plain and went through several cities of the “2 + 26” cities. Fen-wei Plain is one of the key prevention and control areas of air pollution in China. “2 + 26” cities are air pollution transmission channel of Beijing Tianjin Hebei region. Cluster 3 started from the east of Hubei while cluster 4 passed the north of Anhui. Both eastern Hubei and northern Anhui had a high concentration of PM. The ratios of PM2.5 to PM10 associated with cluster 1, 3 and 4 were 0.47, 0.52 and 0.48, respectively. While, the trajectories in cluster 5 had the highest value of PM2.5/PM10as 0.61. Nonetheless, those trajectories had no high pollutant concentration and were not the significant pollution transport pathway.
Table 1
Statistical analysis on trajectories of air flow for each cluster in Hefei City between 2018 and 2020
Season
|
Cluster
|
NTa
|
PNT b (%)
|
PM10c (µg·m− 3)
|
PM2.5c (µg·m− 3)
|
PM2.5/PM10
|
Spring
|
1
|
1035
|
15.22
|
93.37 ± 39.22
|
44.09 ± 19.11
|
0.47
|
|
2
|
1281
|
19.72
|
68.66 ± 30.62
|
39.00 ± 22.52
|
0.57
|
|
3
|
1611
|
23.83
|
81.04 ± 41.80
|
42.41 ± 19.23
|
0.52
|
|
4
|
900
|
13.72
|
89.29 ± 44.17
|
42.77 ± 21.99
|
0.48
|
|
5
|
1228
|
18.84
|
66.62 ± 37.56
|
40.50 ± 22.88
|
0.61
|
|
6
|
563
|
8.67
|
71.60 ± 52.51
|
30.88 ± 16.85
|
0.43
|
Summer
|
1
|
1054
|
15.60
|
53.37 ± 21.56
|
27.44 ± 12.71
|
0.51
|
|
2
|
1888
|
28.84
|
44.00 ± 20.94
|
22.53 ± 9.43
|
0.51
|
|
3
|
1421
|
21.66
|
50.33 ± 21.84
|
26.19 ± 13.63
|
0.52
|
|
4
|
690
|
10.54
|
48.20 ± 24.59
|
23.49 ± 11.89
|
0.49
|
|
5
|
917
|
14.01
|
54.79 ± 27.32
|
26.67 ± 14.10
|
0.49
|
|
6
|
650
|
9.55
|
44.60 ± 22.38
|
21.67 ± 9.84
|
0.49
|
Autumn
|
1
|
279
|
4.32
|
83.22 ± 54.70
|
43.80 ± 25.79
|
0.53
|
|
2
|
727
|
11.26
|
81.01 ± 39.13
|
50.71 ± 35.39
|
0.63
|
|
3
|
1282
|
19.46
|
67.16 ± 33.68
|
33.71 ± 17.70
|
0.50
|
|
4
|
1736
|
26.06
|
73.61 ± 42.12
|
37.08 ± 24.00
|
0.50
|
|
5
|
1797
|
27.83
|
63.07 ± 29.05
|
35.30 ± 18.13
|
0.56
|
|
6
|
715
|
11.07
|
99.40 ± 64.29
|
42.16 ± 27.26
|
0.42
|
Winter
|
1
|
1015
|
15.26
|
89.18 ± 43.19
|
71.11 ± 42.86
|
0.80
|
|
2
|
2041
|
31.83
|
70.67 ± 43.40
|
59.37 ± 40.16
|
0.84
|
|
3
|
1259
|
19.68
|
89.97 ± 47.81
|
72.53 ± 42.14
|
0.81
|
|
4
|
872
|
13.59
|
71.82 ± 36.21
|
70.75 ± 39.39
|
0.99
|
|
5
|
823
|
12.45
|
94.75 ± 40.30
|
69.93 ± 35.48
|
0.74
|
|
6
|
461
|
7.19
|
70.01 ± 45.77
|
70.00 ± 43.66
|
1.00
|
a, number of trajectories
b, percentage of trajectories
c, mean ± std
|
In summer, trajectory values of PM2.5/PM10 among clusters did not obviously vary with the values of ~ 0.50. There were four clusters (1(northwest→east), 3 (east-southeast), 4 (north→east) and 5 (southeast)) with PM10 higher than averaged summer concentration of Hefei while 3 (1,3 and 5) for PM2.5. Cluster 1, 3 and 5 were regarded to be the predominant trajectories that simultaneously affected Hefei’s PM10 and PM2.5. Moreover, the trajectories from cluster 4 were also the major transport pathway that PM10 reached Hefei. Trajectories from clusters 1, 3, 4 and 5 had relationship with the city groups including Shanghai-Suzhou-Wuxi-Changzhou-Nanjing-Maanshan, Jiaxing-Suzhou-Wuxi-Changzhou-Nanjing-Wuhu, Chuzhou-Maanshan-Wuhu and Wenzhou-Lishui-Jinhua-Hangzhou-Huangshan-Chizhou-Tongling, respectively. However, the cluster 2 with the highest percentage of trajectory as 28.84% was not the major pathway of PM migrating to Hefei with heavy pollution.
In autumn, mean trajectory concentrations of PM10 and PM2.5 were 83.22 ± 54.70 and 43.80 ± 25.79 µg·m− 3 in cluster 1, 81.01 ± 39.13 and 50.71 ± 35.39 µg·m− 3 cluster 2, 67.16 ± 33.68 and 33.71 ± 17.70 µg·m− 3 cluster 3, 73.61 ± 42.12 and 37.08 ± 24.00 µg·m− 3 cluster 4, 63.07 ± 29.05 and 35.30 ± 18.13 µg·m− 3 cluster 5 and 99.40 ± 64.29 and 42.16 ± 27.26 µg·m− 3 in cluster 6. As a result, cluster 1, 2, 4 and 6 had the trajectories with high PM10 level while cluster 1, 2 and 6 for PM2.5. The corresponding trajectories of cluster 1, 2, 4 and 6 were observed to pass either Wei-fen plain or “2 + 26” cities. As to PM2.5/PM10, the highest was present in cluster 2 with 0.63 while the smallest from cluster 6 as 0.42.
For winter, the ratio of PM2.5/PM10 in trajectories was significantly higher than that of other seasons. Of those six clusters, cluster 4 and 6 had the highest ratio of around 1.00, while the smallest for cluster 5 as 0.74. And the ratio values of cluster 1, 2 and 3 were 0.80, 0.84 and 0.81. Trajectories of cluster 2, with the highest air mass fraction of 31.83%, were not associated with the concentrations of neither PM10 nor PM2.5 higher than the mean concentration of PM in winter. The highest trajectory concentration of PM appeared at Cluster 5 for PM10 as 94.75 ± 40.30 µg·m− 3 and cluster 3 for PM2.5 as 72.53 ± 42.14 µg·m− 3. Specifically, there were three clusters (1, 3 and 5) containing trajectories with high pollution of PM10 and 5 clusters (1, 3, 4, 5 and 6) for PM2.5. In winter the air mass all passed the places (Wei-fen Plain and “2 + 26” cities) with heavy PM pollution in China.
Figure 7 demonstrates the press profiles of the air mass clustered reaching Hefei. Comparatively, air flow among seasons occurred with the minimum height in summer. In spring the trajectories in cluster 3 with the highest ratio and shortest moving distance were observed to have the smallest height, coupled with pressure of 840 ~ 950 hPa. Meanwhile, the height of those trajectories with the longest transport path changed considerably. Over summer the heights of flow masses in cluster 1 and 6 varied similarly, and decreased gradually. The initial height of trajectories from cluster 4 which had short pathway was the highest. Also those trajectories, derived from the East China Sea, of cluster 3 and 5 almost started at the same height. However, the air flows grouped into cluster 5 was increased and decreased successively as they moved. Coming to autumn, cluster 5 with the highest ratio contained the trajectories with the maximum height. And the height of trajectories in cluster 1 moving with the long way was stable firstly and then rose slightly. Thereafter, it declined dramatically. Regarding winter, the range of initial heights was the smallest among four seasons. And all trajectories had the transport height decreased gradually regardless of cluster. It should be noted that the press profiles were not related with the concentrations of PM in trajectories regardless of season.
[Fig. 7 Pressure profile of back trajectories for air flow in Hefei City between 2018 and 2020]
3.3 Potential contributor sources identification
3.3.1PSCF analysis
WPSCF maps for PM10 and PM2.5 of Hefei City between 2018 and 2020 are provided in Figs. 8 and 9.
[Fig. 8 WPSCF maps for PM10 of Hefei City between 2018 and 2020]
[Fig. 9 WPSCF maps for PM2.5 of Hefei City between 2018 and 2020]
In Spring, PM10’s WPSCF over 0.60 were mainly located in two large zones from 10 provinces (Anhui, Hubei, Hunan, Jiangxi, Zhejiang, Guangxi, Henan, Shanxi, Shaanxi and Huhhot). And the main potential contributors of atmospheric PM10 in Heifei were distributed in the neighboring region of Anhui, Jiangxi and Zhejiang, the middle north of Fujian, the border of Hunan and Hubei, the middle east and south of Hubei, the middle north of Hunan, the border of Shanxi and Henan, etc. Otherwise, the area and value of WPSCF for PM2.5 were smaller than that of PM10 in spring. The significant contributors came from the northeast of Jiangxi, the junction of Anhui, Jiangxi and Zhejiang, the north of Fujian and the northeast of Guangxi, which also could contribute PM10 considerably to Hefei.
In summer, the value of WPSCF, exceeding 0.70, for PM10 mainly appeared in Anhui, Jiangsu and Zhejiang province. And the major cities included Tongling, Xuancheng, Wuhu and Huangshan in Anhui province, Changzhou, Wuxi and Suzhou in Jiangsu province and Huzhou, Jiaxing, Shaoxing, Hangzhou, Quzhou, Jinhua, Lishui in Zhejiang province. Moreover, there were several patches from Jiangxi, Fujian, Shandong and Henan province with WPSCF as 0.70–0.80, being the significant potential contributor. Comparatively, PM2.5’s WPSCF was mainly within the range of < 0.70. And the places, away from the southeast of Hefei, including Tongling, Chizhou, Wuhu, Xuancheng in Anhui province and Huzhou and Hangzhou in Zhejiang Province were recognized as the considerable contributors of PM2.5.
As shown in Fig. 8(c), the sources likely affecting Heifei’ PM10 scattered in Huangshi, Ezhou, Huanggang, Xianning, Suizhou, Jingmen, Shiyan, Nanyang, Sanmenxia, Shangluo,Weinan, Yanan, Yulin and Qingyang Cities. Moreover, there were large areas with WPSC between 0.50 and 0.60 from the middle-lower Yangtze Plain, the Northeast Plain, the Loess Plateau and the Inner Mongolian Plateau. As to PM2.5, its major contributors were from southern Hubei (Xianning and Huanggang) and western Jiangxi (Jiujiang, Yichun and Xinyu). Additionsally, Huaibei, Shangluo, Sanmenxia and Qingyang can also be considered as the significant contributor.
Within winter, WPSC values both of PM10 and PM2.5 the highest of four seasons. The area of PM’s contributors to Hefei was remarkably increased. And the contribution was stronger in northern China than southern China. Specifically, the contributors of PM10 were mainly seated at west, northwest and southwest of Hefei city. The places, between the line of Yinchuang-Zhengzhou city and the line of Zhongwei-Pingdingshan city, covering Henan, Shanxi, Shaanxi and Gansu province, were found to be the significant contributor of PM10 with the largest area. Moreover, northeast Hubei province, southeastern Hubei province, Jianghan Plain and northeast Hunan province were also the strong contributor. On the other hand, PM2.5 was mainly contributed by southeastern Shandong, eastern Henan, northern Anhui, southeastern Hubei, northeast Hunan and southern Shanxi.
3.3.2 WCWT analysis
Figure 10 shows WCWT map distributions of PM10. The results were very similar to that of WPSCF method. In spring the areas with WCWT over 100 µg·m− 3 covering the border of Shanxi and Shaanxi province (Lvliang, Linfen, Yulin and Yanan city), the border of Shanxi and Henan province (Yuncheng, Jincheng, Sanmenxia, Jiyuan, Luoyang and Jiaozuo city), the middle of Henan province (Zhengzhou, Xuchang and Pingdingshan city), the center of Hebei province (Boding city), the junction of Anhui, Jiangxi and Zhejiang province (Huangshan Jingdezheng, Shangrao and Quzhou city). In summer, WCWT was observed in the range of < 70 µg·m− 3. And the places of the south of Anhui province, the south of Jiangsu province and the middle and northern west of Zhejiang province were identified as the main potential contributor. Otherwise, during autumn WCWT of 100–157 µg·m− 3 was found mainly in Henan and Hubei province. Moreover, several patches from Anhui, Shanxi and Shaanxi province were also the significant contributor of PM10. Over winter, there an enormous region with WCWT of PM10 over 90 µg·m− 3. The major contributors were located almost within the whole of Henan province, the middle east of Hubei province, large area of Anhui province, the southwest of Shanxi province, the southwest of Shandong province, west of Zhejiang province, the neighboring region of Hubei, Hunan and Guangxi province as well as the middle of Guangxi province.
[Fig. 10 WCWT maps for PM10 of Hefei City between 2018 and 2020]
WCWT distribution of PM2.5 is given in Fig. 11. The main contributors of PM2.5 with WCWT > 40 µg·m− 3 were widely distributed in the central and eastern China. And the neighboring region of Anhui with Jiangxi and Zhejiang Province, the northwest part of Henan Province, and the middle, northwest and east places of Shandong Province were observed to contribute WCWT as 50 ~ 60 µg·m− 3. Comparatively, summer had the smallest PM2.5 WCWT (< 40 µg·m− 3) among four seasons. And, the areas with WCWT higher than 30 µg·m− 3 were within the large region of southern Anhui province, the north of Zhejiang province and the south of Jiangsu province. Into autumn, the contribution area of PM2.5 started to expand with WCWC mainly as 40 ~ 70 µg·m− 3. Over winter, WCWT of 90 ~ 100 µg·m− 3 was concentrated at the southeast of Hubei Province, the east of Henan Province and the southwest of Shandong Province.
[Fig. 11 WCWT maps for PM2.5 of Hefei City between 2018 and 2020]
As above-discussed, the potential contributor sources to Hefei city seasonally varied. And the places from Shanxi, Hebei, Henan and Anhui Province were identified as the major contributor. Dring 2001 ~ 2005, dust storm episode could significantly affect Hefei’s PM concentration, especially in spring [22]. Interestingly, inner Mongolia where dust storm episode frequently previously did not seem to be the important contributor by the present study. A study by Yu et al. [23] shows that Anqing, a neighboring city of Hefei, was mainly contributed by the sources from the east of Hubei province, north of Jiangxi province and south of Hunan province, which was coupled with a planar area involved in Shanxi, Henan, southern Shandong and northern Anhui province. And there are several places as the same contributor to both Anqing and Hefei.