{"title":"[PM2.5 中水溶性离子污染特征及大连 PM2.5 酸度较高的原因]。","authors":"Meng Yang, Chang Liu, Xiao-Huan Wang, Lian-Lian Liu, Ming-Ming Zhang, Shan-Shan Cao, Shou-Zheng Yan, Ze-Yu Sun, Chong-Guo Tian","doi":"10.13227/j.hjkx.202309149","DOIUrl":null,"url":null,"abstract":"<p><p>To gain a deeper understanding of the pollution status and influencing factors of fine particles (PM<sub>2.5</sub>) and their water-soluble ions (WSI) in Dalian and to implement precise control of pollution events such as haze and acid rain, PM<sub>2.5</sub> samples were collected in Dalian from June 2021 to May 2022. Then, the mass concentrations of PM<sub>2.5</sub> and WSI were determined using the weight method and ion chromatography, respectively, and the pollution characteristics and sources were analyzed. Furthermore, the causes of the high acidity of PM<sub>2.5</sub> in spring were discussed. The results showed that the annual average mass concentrations of PM<sub>2.5</sub> and WSI in Dalian during the sampling period were (33.24 ±28.87) μg·m<sup>-3</sup> and (18.66 ±20.52) μg·m<sup>-3</sup>, respectively, and the secondary ions (SNA, including SO<sub>4</sub><sup>2-</sup>, NO<sub>3</sub><sup>-</sup>, and NH<sub>4</sub><sup>+</sup>) accounted for the highest proportion of WSI [(86.2 ±9.3)%]. The order of ion concentration levels from highest to lowest was: NO<sub>3</sub><sup>-</sup>>SO<sub>4</sub><sup>2-</sup>>NH<sub>4</sub><sup>+</sup>>Cl<sup>-</sup>>K<sup>+</sup>>Ca<sup>2+</sup>>Na<sup>+</sup>>Mg<sup>2+</sup>>F<sup>-</sup>. Due to the influence of meteorological conditions and coal combustion emissions during the concentrated heating period from late autumn to early spring, the seasonal variation in PM<sub>2.5</sub> and WSI was winter>spring>autumn>summer, whereas SNA was the highest in spring and the lowest in summer. The results of correlation and principal component analysis showed that WSI in PM<sub>2.5</sub> was mainly from the secondary transformation of atmospheric SO<sub>2</sub> and NO<sub>2</sub> (contributing to the majority of SNA), mixed sources of combustion and dust (characterized by K<sup>+</sup>, Mg<sup>2+</sup>, Cl<sup>-</sup>, and F<sup>-</sup>), and sources of sand and sea salt (characterized by Na<sup>+</sup>, Ca<sup>2+</sup>, and Mg<sup>2+</sup>). In summer, the main combustion source was biomass burning, whereas in autumn, winter, and spring, coal combustion emissions were predominant. The change in wind direction from autumn to winter brought by a shift from the source of sea salt to soil dust; additionally, the external pollution transported by northwest winds contributed to the complexity of the sources of WSI in PM<sub>2.5</sub> during spring in Dalian. ISORROPIA-II model simulations suggested NH<sub>4</sub>NO<sub>3</sub> as the most present solid aerosol form in PM<sub>2.5</sub> in Dalian, followed by CaSO<sub>4</sub> and (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub>; compared to that in solid aerosols, more SNA existed in liquid aerosols. The annual average pH of PM<sub>2.5</sub> in Dalian was 5.65 ±3.00, with pH values close to neutral in summer, autumn, and winter but significantly acidic in spring (2.03 ±3.18). The high acidity observed in spring was attributed to the combination of low temperature, high humidity, and high SNA concentrations. These conditions resulted in higher aerosol water content and increased gas-to-particle conversion rates, ultimately leading to an ammonia-deficient environment. The backward trajectory and PSCF results indicated that the external transport of high acidity PM<sub>2.5</sub> in spring mainly came from the northwest (45.0%) and southwest (40.8%) directions. Mobile source emissions made the most significant contribution to the transportation of pollutants in the former, forming high-pollution source areas in the Beijing-Tianjin-Hebei Region, which may have been mainly related to urban motor vehicle and port vessel emissions; the latter was influenced by relatively strong stationary sources and showed higher SO<sub>2</sub> emissions in the southern part of Henan Province and the central part of Jiangsu Province.</p>","PeriodicalId":35937,"journal":{"name":"Huanjing Kexue/Environmental Science","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"[Characteristics of Water-soluble Ion Pollution in PM<sub>2.5</sub> and the Causes of High Acidity of PM<sub>2.5</sub> in Dalian].\",\"authors\":\"Meng Yang, Chang Liu, Xiao-Huan Wang, Lian-Lian Liu, Ming-Ming Zhang, Shan-Shan Cao, Shou-Zheng Yan, Ze-Yu Sun, Chong-Guo Tian\",\"doi\":\"10.13227/j.hjkx.202309149\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>To gain a deeper understanding of the pollution status and influencing factors of fine particles (PM<sub>2.5</sub>) and their water-soluble ions (WSI) in Dalian and to implement precise control of pollution events such as haze and acid rain, PM<sub>2.5</sub> samples were collected in Dalian from June 2021 to May 2022. Then, the mass concentrations of PM<sub>2.5</sub> and WSI were determined using the weight method and ion chromatography, respectively, and the pollution characteristics and sources were analyzed. Furthermore, the causes of the high acidity of PM<sub>2.5</sub> in spring were discussed. The results showed that the annual average mass concentrations of PM<sub>2.5</sub> and WSI in Dalian during the sampling period were (33.24 ±28.87) μg·m<sup>-3</sup> and (18.66 ±20.52) μg·m<sup>-3</sup>, respectively, and the secondary ions (SNA, including SO<sub>4</sub><sup>2-</sup>, NO<sub>3</sub><sup>-</sup>, and NH<sub>4</sub><sup>+</sup>) accounted for the highest proportion of WSI [(86.2 ±9.3)%]. The order of ion concentration levels from highest to lowest was: NO<sub>3</sub><sup>-</sup>>SO<sub>4</sub><sup>2-</sup>>NH<sub>4</sub><sup>+</sup>>Cl<sup>-</sup>>K<sup>+</sup>>Ca<sup>2+</sup>>Na<sup>+</sup>>Mg<sup>2+</sup>>F<sup>-</sup>. Due to the influence of meteorological conditions and coal combustion emissions during the concentrated heating period from late autumn to early spring, the seasonal variation in PM<sub>2.5</sub> and WSI was winter>spring>autumn>summer, whereas SNA was the highest in spring and the lowest in summer. The results of correlation and principal component analysis showed that WSI in PM<sub>2.5</sub> was mainly from the secondary transformation of atmospheric SO<sub>2</sub> and NO<sub>2</sub> (contributing to the majority of SNA), mixed sources of combustion and dust (characterized by K<sup>+</sup>, Mg<sup>2+</sup>, Cl<sup>-</sup>, and F<sup>-</sup>), and sources of sand and sea salt (characterized by Na<sup>+</sup>, Ca<sup>2+</sup>, and Mg<sup>2+</sup>). In summer, the main combustion source was biomass burning, whereas in autumn, winter, and spring, coal combustion emissions were predominant. The change in wind direction from autumn to winter brought by a shift from the source of sea salt to soil dust; additionally, the external pollution transported by northwest winds contributed to the complexity of the sources of WSI in PM<sub>2.5</sub> during spring in Dalian. ISORROPIA-II model simulations suggested NH<sub>4</sub>NO<sub>3</sub> as the most present solid aerosol form in PM<sub>2.5</sub> in Dalian, followed by CaSO<sub>4</sub> and (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub>; compared to that in solid aerosols, more SNA existed in liquid aerosols. The annual average pH of PM<sub>2.5</sub> in Dalian was 5.65 ±3.00, with pH values close to neutral in summer, autumn, and winter but significantly acidic in spring (2.03 ±3.18). The high acidity observed in spring was attributed to the combination of low temperature, high humidity, and high SNA concentrations. These conditions resulted in higher aerosol water content and increased gas-to-particle conversion rates, ultimately leading to an ammonia-deficient environment. The backward trajectory and PSCF results indicated that the external transport of high acidity PM<sub>2.5</sub> in spring mainly came from the northwest (45.0%) and southwest (40.8%) directions. Mobile source emissions made the most significant contribution to the transportation of pollutants in the former, forming high-pollution source areas in the Beijing-Tianjin-Hebei Region, which may have been mainly related to urban motor vehicle and port vessel emissions; the latter was influenced by relatively strong stationary sources and showed higher SO<sub>2</sub> emissions in the southern part of Henan Province and the central part of Jiangsu Province.</p>\",\"PeriodicalId\":35937,\"journal\":{\"name\":\"Huanjing Kexue/Environmental Science\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-09-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Huanjing Kexue/Environmental Science\",\"FirstCategoryId\":\"1087\",\"ListUrlMain\":\"https://doi.org/10.13227/j.hjkx.202309149\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"Environmental Science\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Huanjing Kexue/Environmental Science","FirstCategoryId":"1087","ListUrlMain":"https://doi.org/10.13227/j.hjkx.202309149","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"Environmental Science","Score":null,"Total":0}
引用次数: 0
摘要
深入了解细颗粒物(PM2.5)及其水溶性离子(WSI)的污染状况和影响因素。及其水溶性离子(WSI)为准确了解大连市细颗粒物(PM2.5)及其水溶性离子(WSI)的污染状况,对雾霾、酸雨等污染事件实施精准控制,2021年6月至2022年5月在大连市采集了PM2.5样品。然后,分别采用重量法和离子色谱法测定了 PM2.5 和 WSI 的质量浓度,分析了污染特征和污染源。此外,还讨论了春季 PM2.5 酸度较高的原因。结果表明,采样期间大连市 PM2.5 和 WSI 的年均质量浓度分别为(33.24 ±28.87)μg-m-3和(18.66 ±20.52)μg-m-3。μg-m-3)和(18.66±20.52)μg-m-3),二次离子(SNA,包括SO42-、NO3-和NH4+)在WSI中所占比例最高。占 WSI 的比例最高[(86.2 ±9.3)%]。离子浓度从高到低的顺序为:NO3->SO42->NH4+>Cl->K+>Ca2+>Na+>Mg2+>F-。由于受气象条件和秋末至初春集中采暖期燃煤排放的影响,PM2.5和WSI的季节变化为冬季>春季>秋季>夏季,而SNA则以春季最高,夏季最低。相关分析和主成分分析结果表明,PM2.5 中的 WSI 主要来自于 PM2.5 的二次转化。5中的WSI主要来自大气中SO2和NO2的二次转化(占SNA的大部分)、燃烧和粉尘的混合源(以K+、Mg2+、Cl-和F-为特征)以及沙尘和海盐源(以Na+、Ca2+和Mg2+为特征)。夏季的主要燃烧源是生物质燃烧,而秋季、冬季和春季则以燃煤排放为主。从秋季到冬季,风向的变化带来了海盐源向土壤尘源的转移;此外,西北风带来的外部污染也导致了大连春季 PM2.5 中 WSI 来源的复杂性。ISORROPIA-II模型模拟表明,大连PM2.5中存在最多的固体气溶胶形式是NH4NO3,其次是CaSO4和(NH4)2SO4;与固体气溶胶相比,液态气溶胶中存在更多的SNA。大连 PM2.5 的年平均 pH 值为 5.65 ±3.00,夏季、秋季和冬季的 pH 值接近中性,但春季的 pH 值明显偏酸(2.03 ±3.18)。春季的高酸度是由于低温、高湿度和高 SNA 浓度共同造成的。这些条件导致气溶胶含水量升高,气体到粒子的转化率增加,最终形成了缺氨环境。后向轨迹和PSCF结果表明,春季高酸度PM2.5的外部输送主要来自西北(45.0%)和西南(40.8%)。和西南方向(40.8%)。方向。移动源排放对前者污染物的输送贡献最大,在京津冀地区形成高污染源区,可能主要与城市机动车和港口船舶排放有关;后者受固定源影响相对较强,在河南省南部和江苏省中部地区SO2排放量较高。
[Characteristics of Water-soluble Ion Pollution in PM2.5 and the Causes of High Acidity of PM2.5 in Dalian].
To gain a deeper understanding of the pollution status and influencing factors of fine particles (PM2.5) and their water-soluble ions (WSI) in Dalian and to implement precise control of pollution events such as haze and acid rain, PM2.5 samples were collected in Dalian from June 2021 to May 2022. Then, the mass concentrations of PM2.5 and WSI were determined using the weight method and ion chromatography, respectively, and the pollution characteristics and sources were analyzed. Furthermore, the causes of the high acidity of PM2.5 in spring were discussed. The results showed that the annual average mass concentrations of PM2.5 and WSI in Dalian during the sampling period were (33.24 ±28.87) μg·m-3 and (18.66 ±20.52) μg·m-3, respectively, and the secondary ions (SNA, including SO42-, NO3-, and NH4+) accounted for the highest proportion of WSI [(86.2 ±9.3)%]. The order of ion concentration levels from highest to lowest was: NO3->SO42->NH4+>Cl->K+>Ca2+>Na+>Mg2+>F-. Due to the influence of meteorological conditions and coal combustion emissions during the concentrated heating period from late autumn to early spring, the seasonal variation in PM2.5 and WSI was winter>spring>autumn>summer, whereas SNA was the highest in spring and the lowest in summer. The results of correlation and principal component analysis showed that WSI in PM2.5 was mainly from the secondary transformation of atmospheric SO2 and NO2 (contributing to the majority of SNA), mixed sources of combustion and dust (characterized by K+, Mg2+, Cl-, and F-), and sources of sand and sea salt (characterized by Na+, Ca2+, and Mg2+). In summer, the main combustion source was biomass burning, whereas in autumn, winter, and spring, coal combustion emissions were predominant. The change in wind direction from autumn to winter brought by a shift from the source of sea salt to soil dust; additionally, the external pollution transported by northwest winds contributed to the complexity of the sources of WSI in PM2.5 during spring in Dalian. ISORROPIA-II model simulations suggested NH4NO3 as the most present solid aerosol form in PM2.5 in Dalian, followed by CaSO4 and (NH4)2SO4; compared to that in solid aerosols, more SNA existed in liquid aerosols. The annual average pH of PM2.5 in Dalian was 5.65 ±3.00, with pH values close to neutral in summer, autumn, and winter but significantly acidic in spring (2.03 ±3.18). The high acidity observed in spring was attributed to the combination of low temperature, high humidity, and high SNA concentrations. These conditions resulted in higher aerosol water content and increased gas-to-particle conversion rates, ultimately leading to an ammonia-deficient environment. The backward trajectory and PSCF results indicated that the external transport of high acidity PM2.5 in spring mainly came from the northwest (45.0%) and southwest (40.8%) directions. Mobile source emissions made the most significant contribution to the transportation of pollutants in the former, forming high-pollution source areas in the Beijing-Tianjin-Hebei Region, which may have been mainly related to urban motor vehicle and port vessel emissions; the latter was influenced by relatively strong stationary sources and showed higher SO2 emissions in the southern part of Henan Province and the central part of Jiangsu Province.