贵阳秋季PM_(2.5)水溶性离子组成特征及来源解析
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摘要
水溶性无机离子是PM_(2.5)的主要组分之一,对研究PM_(2.5)的物理化学性质,来源及其形成机理具有重要意义.本研究于2017年9月—2017年11月期间在贵阳城区采集了80个PM_(2.5)样品,并测定了8种水溶性离子浓度,探讨贵阳秋季PM_(2.5)水溶性离子组成特征及来源.结果表明贵阳秋季PM_(2.5)中无机离子的平均质量浓度为15.99μg·m~(-3),阴离子和阳离子的平均质量浓度分别为10. 90μg·m~(-3)、5. 09μg·m~(-3); SO_4~(2-)(8. 53±4.63μg·m~(-3))平均质量浓度最高,其次是NH_4~+(2.56±1.62μg·m~(-3))、NO_3~-(2.21±2.96μg·m~(-3))、Ca~(2+)(1.98±0.88μg·m~(-3)),最后依次是K~+(0.37±0.24μg·m~(-3))、Cl-(0.16±0.11μg·m~(-3))、Mg~(2+)(0.11±0.03μg·m~(-3))、Na~+(0.07±0.06μg·m~(-3)); NH_4~+、SO_4~(2-)、NO_3~-是主要水溶性离子,所占比例为83%; NO_3~-/SO_4~(2-)值平均为0.21±0.12,远小于1,说明贵阳秋季PM_(2.5)以固定源污染为主.相关性分析表明,PM_(2.5)中NH_4~+主要以(NH_4)_2SO_4、NH_4HSO_4、NH_4NO_3的形式存在,Ca~(2+)与Mg~(2+)来源可能相同.结合富集系数分析NO_3~-、SO_4~(2-)、Ca~(2+)、K~+、Mg~(2+)基本都是来源于陆源贡献,NO_3~-、SO_4~(2-)是人为源,Ca~(2+)、K~+、Mg~(2+)是地壳源,此外Mg~(2+)还有一部分海源贡献.
Composition analysis of water-soluble ions( WSIs) in fine particulate aerosol is of great significance for understanding the physical and chemical characteristics,sources and formation mechanism of PM_(2.5). In the present study,a total of eighty PM_(2.5) samples were collected in Guiyang urban area from September to November, 2017. Eight water-soluble ions were deterained to investigate the composition and sources of PM_(2.5) water-soluble ions during autumn in Guiyang.Results showed that the average concentration of inorganic ions was 15. 99 μg·m~(-3),while the averaged mass concentrations of anions and cations were respectively 10. 90 μg·m~(-3) and 5.09 μg·m~(-3). Among the interested ionic species,SO_4~(2-)( 8. 53 ± 4. 63 μg·m~(-3)) was the highest,followed by NH_4~+( 2.56±1.62 μg·m~(-3)),NO_3~-( 2.21±2.96 μg·m~(-3)) and Ca~(2+)( 1.98±0.88 μg·m~(-3)),while other ions ranked as K~+( 0. 37 ± 0. 24 μg·m~(-3)),Cl-( 0. 16 ± 0. 11 μg·m~(-3)),Mg~(2+) ( 0. 11 ±0.03 μg·m~(-3)) 、Na~+( 0.07±0.06 μg·m~(-3)). In general,NH_4~+,SO_4~(2-) and NO_3~- were the main watersoluble ions,accounting for 83% of total inorganic ions. The ratio of NO_3~-/SO_4~(2-)( 0.21±0.12) was much lower than unit,indicating that Guiyang PM_(2.5) mainly suffered stationary source pollution during the sampling time. The correlation analysis showed that most of NH_4~+ existed in the form of(NH_4)_2SO_4,NH_4HSO_4 and NH_4NO_3 in PM_(2.5). Enrichment factor analysis relative to seawater and soil indicated that NO_3~-,SO_4~(2-),Ca~(2+),K~+,and Mg~(2+) were basically derived from terrestrial sources,while SO_4~(2-) and NO_3~- were from the anthropogenic source,Ca~(2+),K~+,and Mg~(2+) mainly from crustal sources,a part of Mg~(2+) was from the sea source.
Composition analysis of water-soluble ions( WSIs) in fine particulate aerosol is of great significance for understanding the physical and chemical characteristics,sources and formation mechanism of PM_(2.5). In the present study,a total of eighty PM_(2.5) samples were collected in Guiyang urban area from September to November, 2017. Eight water-soluble ions were deterained to investigate the composition and sources of PM_(2.5) water-soluble ions during autumn in Guiyang.Results showed that the average concentration of inorganic ions was 15. 99 μg·m~(-3),while the averaged mass concentrations of anions and cations were respectively 10. 90 μg·m~(-3) and 5.09 μg·m~(-3). Among the interested ionic species,SO_4~(2-)( 8. 53 ± 4. 63 μg·m~(-3)) was the highest,followed by NH_4~+( 2.56±1.62 μg·m~(-3)),NO_3~-( 2.21±2.96 μg·m~(-3)) and Ca~(2+)( 1.98±0.88 μg·m~(-3)),while other ions ranked as K~+( 0. 37 ± 0. 24 μg·m~(-3)),Cl-( 0. 16 ± 0. 11 μg·m~(-3)),Mg~(2+) ( 0. 11 ±0.03 μg·m~(-3)) 、Na~+( 0.07±0.06 μg·m~(-3)). In general,NH_4~+,SO_4~(2-) and NO_3~- were the main watersoluble ions,accounting for 83% of total inorganic ions. The ratio of NO_3~-/SO_4~(2-)( 0.21±0.12) was much lower than unit,indicating that Guiyang PM_(2.5) mainly suffered stationary source pollution during the sampling time. The correlation analysis showed that most of NH_4~+ existed in the form of(NH_4)_2SO_4,NH_4HSO_4 and NH_4NO_3 in PM_(2.5). Enrichment factor analysis relative to seawater and soil indicated that NO_3~-,SO_4~(2-),Ca~(2+),K~+,and Mg~(2+) were basically derived from terrestrial sources,while SO_4~(2-) and NO_3~- were from the anthropogenic source,Ca~(2+),K~+,and Mg~(2+) mainly from crustal sources,a part of Mg~(2+) was from the sea source.
引文
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[3] XIAO H W, XIAO H Y, LUO L, et al. Atmospheric aerosol compositions over the South China Sea: Temporal variability and source apportionment[J]. Atmospheric Chemistry & Physics, 2017, 17(4): 3199-3214.
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[6] FONTES T, LI P, BARROS N, et al. Trends of PM2.5 concentrations in China: A long term approach[J]. Journal of Environmental Management, 2017, 196(2): 719-732.
[7] TAN J, DUAN J, ZHEN N, et al. Chemical characteristics and source of size-fractionated atmospheric particle in haze episode in Beijing[J]. Atmospheric Research, 2016, 167: 24-33.
[8] TAO J, CHENG T T, ZHANG R J. Chemical composition of summertime PM and its relationship to aerosol optical properties in Guangzhou, China[J]. Atmospheric & Oceanic Science Letters, 2015, 5(2): 88-94.
[9] LI L, WU W, FENG J, et al. Composition, source, mass closure of PM2.5 aerosols for four forests in eastern China[J]. Journal of Environmental Science (English), 2010, 22(3): 405-412.
[10] ZHAO P S, DONG F, HE D, et al. Characteristics of concentrations and chemical compositions for PM2.5 in the region of Beijing, Tianjin, and Hebei, China[J]. Atmospheric Chemistry & Physics, 2013, 13(1): 4631-4644.
[11] TAO J, GAO J, ZHANG L, et al. PM2.5 pollution in a megacity of southwest China: Source apportionment and implication[J]. Atmospheric Chemistry & Physics, 2014, 14(4): 8679-8699.
[12] 贵阳市统计局. 贵阳统计年鉴(2002-2016)[M]. 北京:中国统计出版社,2002-2016.Guiyang Municipal Bureau of Statistics. Guiyang Statistical Yearbook (2002-2016) [M]. Beijing: China Statistics Press, 2002-2016(in Chinese).
[13] XIAO H W, XIAO H Y, LONG A M, et al. Who controls the monthly variations of NH+4 nitrogen isotope composition in precipitation?[J]. Atmospheric Environment, 2012, 54(5): 201-206.
[14] XIAO H Y, LIU C Q. Chemical characteristics of water-soluble components in TSP over Guiyang, SW China, 2003[J]. Atmospheric Environment, 2004, 38(37): 6297-6306.
[15] XIAO H W, XIAO H Y, LONG A M, et al. Chemical composition and source apportionment of rainwater at Guiyang, SW China[J]. Journal of Atmospheric Chemistry, 2013, 70(3): 269-281.
[16] XIE R K, SEIP H M, LEINUM J R, et al. Chemical characterization of individual particles (PM10) from ambient air in Guiyang City, China[J]. Science of the Total Environment, 2005, 343(1-3): 261-272.
[17] CHOW J C, FUJITA E M, WATSON J G, et al. Evaluation of filter-based aerosol measurements during the 1987 southern california air quality study[J]. Environmental Monitoring & Assessment, 1994, 30(1): 49-80.
[18] 肖红伟, 肖化云, 唐从国, 等. 贵阳地区氨排放量估算[J]. 地球与环境, 2010, 38(1): 21-25.XIAO H W, XIAO H Y, TANG C G, et al. Estimation of ammonia emission in Guiyang City[J]. Earth and Environment, 2010, 38(1): 21-25(in Chinese).
[19] 刘学炎, 肖化云, 刘丛强, 等. 贵阳地区主要大气氮源的沉降机制与分布:基于石生苔藓氮含量和氮同位素的证据[J]. 地球化学, 2008, 37(5): 455-461.LIU X Y, XIAO H Y, LIU C Q, et al. Deposition mechanism and distribution of the dominating atmospheric N sources in Guiyang area: Evidences from tissue N and δ15N in epilithic mosses[J]. Geochimica, 2008, 37(5): 455-461(in Chinese).
[20] 李建文, 毕丽玫, 韩新宇,等. 昆明市PM2.5中水溶性无机离子时空变化特征及来源分析[J]. 云南大学学报(自然科学版), 2017, 39(1): 63-70.LI J W, BI L M, HAN X Y, et al. Characteristics and source apportionment of the water soluble inorganic ions in PM2.5 of Kunming[J]. Journal of Yunnan University (Natural Sciences Edition), 2017, 39(1): 63-70 (in Chinese)
[21] HE Q, YAN Y, GUO L, et al. Characterization and source analysis of water-soluble inorganic ionic species in PM2.5 in Taiyuan City, China[J]. Atmospheric Research, 2017, 184: 48-55.
[22] YIN L, NIU Z, CHEN X, et al. Characteristics of water-soluble inorganic ions in PM2.5 and PM2.5-10 in the coastal urban agglomeration along the Western Taiwan Strait Region, China[J]. Environ Sci Pollut Res Int, 2014, 21(7): 5141-5156.
[23] THEODOSI C, GRIVAS G, ZARMPAS P, et al. Mass and chemical composition of size-segregated aerosols (PM1, PM2.5, PM10) over Athens, Greece: Local versus regional sources[J]. Atmospheric Chemistry & Physics & Discussions, 2011, 11(22): 11895-11911.
[24] BRESSI M, SCIARE J, GHERSI V, et al. A one-year comprehensive chemical characterisation of fine aerosol (PM2.5) at urban, suburban and rural background sites in the region of Paris (France)[J]. Atmospheric Chemistry & Physics Discussions, 2013, 13(15): 7825-7844.
[25] SUNDER R R, HOPKE P K, HOLSEN T M. Characterization of fine aerosol and its inorganic components at two rural locations in New York State[J]. Environmental Monitoring & Assessment, 2008, 144(1-3): 351-366.
[26] 肖红伟, 肖化云, 王燕丽. 贵阳大气降水化学特征及来源分析[J]. 中国环境科学, 2010, 30(12): 1590-1596.XIAO H W, XIAO H Y, WANG Y L. Chemical characteristics and source apportionment of precipitation in Guiyang[J]. China Environmental Science, 2010, 30(12): 1590-1596 (in Chinese).
[27] 李友谊, 肖化云, 刘学炎,等. 贵阳市大气总悬浮颗粒物(TSP)中水溶性无机离子的化学特性及季节变化特征[J]. 矿物岩石地球化学通报, 2008, 27(1): 43-49.LI Y Y, XIAO H Y, LIU X Y, et al. Chemical characteristics and seasonal variation of water-soluble inorganic ions in TSP in Guiyang, SW China[J]. Bulletin of Mineralogy,Petrology and Geochemistry, 2008, 27(1): 43-49 (in Chinese).
[28] 孙广权, 李金娟, 陶芸,等. 都匀PM10中水溶性无机离子分布特征与来源分析[J]. 环境监测管理与技术, 2015, 27(6): 13-16.SUN G Q, LI J J,TAO Y, et al. Distribution characteristics and sources analysis of water-soluble inorganic ions in PM10 in Duyun City[J]. The Administration and Technique of Environmental Monitoring, 2015, 27(6): 13-16 (in Chinese).
[29] ARIMOTO R, DUCE R A, SAVOIE D L, et al. Relationships among aerosol constituents from Asia and the North Pacific during PEM‐West A[J]. Journal of Geophysical Research Atmospheres, 1996, 101(D1): 2011-2023.
[30] YAO X, CHAN C K, FANG M, et al. The water-soluble ionic composition of PM2.5 in Shanghai and Beijing, China[J]. Atmospheric Environment, 2002, 36(26): 4223-4234.
[31] HUEBERT B J, WANG M X, WEI-XIU L. Atmospheric nitrate, sulfate, ammonium and calcium concentrations in China[J]. Tellus Series B-chemical & Physical Meteorology, 1988, 40B(4): 260-269.
[32] MING L, JIN L, LI J, et al. PM2.5 in the Yangtze River Delta, China: Chemical compositions, seasonal variations, and regional pollution events[J]. Environmental Pollution, 2017, 223: 200-212.
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