武汉市大气PM_(2.5)主要水溶性离子的时空污染特征
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摘要
目的研究武汉市大气PM_(2.5)主要水溶性离子的时空污染特征。方法 2016年1—12月连续对武汉市5个监测点进行PM_(2.5)采样,用离子色谱法分析其主要水溶性离子成分,并对季节性变化和空间分布差异进行分析。结果武汉市PM_(2.5)质量浓度季节性变化明显。Cl~-季节性趋势不明显,其他离子质量浓度和占比的季节性差异较大。空间分布上,5个监测点均为SO_4~(2-)质量浓度最高,NO~-_3和NH~+_4次之,Cl~-最低,但武昌区和青山区的总离子质量浓度较大,江岸区质量浓度最低;离子的占比存在一致性,即SO■占比远大于其他离子,Cl~-最低,NO~-_3和NH~+_4相当。全年PM_(2.5)的酸碱度R值为0.83,呈酸性;NOR趋势为冬>秋>春>夏,SOR趋势为夏天最高,冬天最低。NO~-_3/SO_4~(2-)季节性变化明显,年均值<1,说明大气中硫和氮主要来源于固定源。结论武汉市大气PM_(2.5)主要水溶性离子(SO■,NO~-_3,NH~+_4)季节性差异明显,空间分布也有差异。
Objectives To investigate the temporal and spatial pollution characteristics of major water-soluble ions in atmospheric PM_(2.5) in Wuhan. Methods For the whole year of 2016 from January to December, PM_(2.5) was continuously sampled from 5 monitoring sites in Wuhan, and the main water-soluble ions in PM_(2.5) were analyzed via Ion Chromatography. The seasonal variation and spatial distribution difference were also examined in this study. Results It showed obvious seasonal variations on PM_(2.5) mass concentration in Wuhan. Meanwhile, the mass concentration and proportion of other ions(except for Cl~-) in PM_(2.5) also had obvious seasonal variation. From the perspective of spatial distribution, the SO■ concentration was the highest in all 5 monitoring sites, followed by NO~-_3 and NH~+_4 and Cl~- concentration was the lowest. However, the total ion concentrations in Wuchang district and Qingshan district were relatively higher, while the concentration in Jiang'an district was the lowest. The ion proportions were consistent, that is, the proportion of SO■ was much larger than that of other ions. Cl~- was the lowest, and NO_3~- and NH_4~+ were at the same level. The acidity of PM_(2.5)showed that PM_(2.5) was acidic all over the year(R=0.83). The NOR trend was: winter > autumn > spring > summer, and the SOR trend was the highest value appeared in summer and lowest value appeared in winter. The seasonal variation of NO~-_3/SO■ was obvious with an annual average <1, indicating that sulfur and nitrogen in the atmosphere are mainly from stationary sources. Conclusions The major water-soluble ions in atmospheric PM_(2.5) in Wuhan showed obvious seasonal variations and spatial distribution variations.
Objectives To investigate the temporal and spatial pollution characteristics of major water-soluble ions in atmospheric PM_(2.5) in Wuhan. Methods For the whole year of 2016 from January to December, PM_(2.5) was continuously sampled from 5 monitoring sites in Wuhan, and the main water-soluble ions in PM_(2.5) were analyzed via Ion Chromatography. The seasonal variation and spatial distribution difference were also examined in this study. Results It showed obvious seasonal variations on PM_(2.5) mass concentration in Wuhan. Meanwhile, the mass concentration and proportion of other ions(except for Cl~-) in PM_(2.5) also had obvious seasonal variation. From the perspective of spatial distribution, the SO■ concentration was the highest in all 5 monitoring sites, followed by NO~-_3 and NH~+_4 and Cl~- concentration was the lowest. However, the total ion concentrations in Wuchang district and Qingshan district were relatively higher, while the concentration in Jiang'an district was the lowest. The ion proportions were consistent, that is, the proportion of SO■ was much larger than that of other ions. Cl~- was the lowest, and NO_3~- and NH_4~+ were at the same level. The acidity of PM_(2.5)showed that PM_(2.5) was acidic all over the year(R=0.83). The NOR trend was: winter > autumn > spring > summer, and the SOR trend was the highest value appeared in summer and lowest value appeared in winter. The seasonal variation of NO~-_3/SO■ was obvious with an annual average <1, indicating that sulfur and nitrogen in the atmosphere are mainly from stationary sources. Conclusions The major water-soluble ions in atmospheric PM_(2.5) in Wuhan showed obvious seasonal variations and spatial distribution variations.
引文
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[8] 刀谞,张霖琳,王超,等.京津冀冬季与夏季PM2.5/PM10及其水溶性离子组分区域性污染特征分析[J].环境化学,2015,34(1):60-69.(In English:Dao X,Zhang LL,Wang C,et al.Characteristics of mass and ionic compounds of atmospheric particles in winter and summer of Beijing-Tianjin-Hebei area,China[J].Environ Chem,2015,34(1):60-69.)
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[10] 葛顺,汤莉莉,秦玮,等.南京地区秋季灰霾天气特征及其水溶性离子分析[J].环境科学与技术,2015,38(2):99-104.(In English:Ge S,Tang LL,Qin W,et al.Characteristics analysis of haze and water-soluble ion in Nanjing in Autumn[J].Environ Sci Technol,2015,38(2):99-104.)
[11] Long SL,Zeng JR,Li Y,et al.Characteristics of secondary inorganic aerosol and sulfate species in size -fractionated aerosol particles in Shanghai[J].J Environ Sci,2014,26(5):1040-1051.
[12] 孟晓艳,余予,张志富,等.2013年1月京津冀地区强雾霾频发成因初探[J].环境科学与技术,2014,37(1):190-194.(In English:Meng XY,Yu Y,Zhang ZF,et al.Preliminary study of the dense fog and haze events' formation over Beijing-Tianjin-and-Hebei region in January of 2013[J].Environ Sci Technol,2014,37(1):190-194.)
[13] Xu LL,Chen XQ,Chen JS,et al.Seasonal variations and chemical compositions of PM2.5 aerosol in the urban area of Fuzhou,China[J].Atmos Res,2012,104-105:264-272.
[14] 范美益,曹芳,张园园,等.徐州市冬季大气细颗粒物水溶性无机离子污染特征及来源解析[J].环境科学,2017,38(11):4478-4485.(In English:Fan MY,Cao F,Zhang YY,et al.Characteristics and sources of water soluble inorganic ions in fine particulate matter during winter in Xuzhou[J].Environ Sci,2017,38(11):4478-4485.)
[15] 王晓琦,周颖,程水源,等.典型城市冬季PM2.5水溶性离子污染特征与传输规律研究[J].中国环境科学,2016,36(8):2289-2296.(In English:Wang XQ,Zhou Y,Cheng SY,et al.Characterization and regional transmission impact of water-soluble ions in PM2.5 during winter in typical cities[J].China Environ Sci,2016,36(8):2289-2296.)
[16] 魏巧珍,王宇红,李盛,等.基于PCA-MLR模型的兰州市大气PM2.5污染来源解析[J].环境卫生学杂志,2017,7(4):267-273.(In English:Wei QZ,Wang YH,Li S,et al.The source apportionment of PM2.5 based on PCA-MLR model in Lanzhou City[J].J Environ Hyg,2017,7(4):267-273.)
[17] 幸娇萍,邵龙义,李红,等.北京灰霾天PM2.5中有机官能团和无机离子的ATR-FTIR研究[J].中国环境科学,2016,36(6):1654-1659.(In English:Xing JP,Shao LY,Li H,et al.ATR-FTIR characterization of organic functional groups and inorganic ions of the haze PM2.5 in Beijing[J].China Environ Sci,2016,36(6):1654-1659.)
[18] 闫广轩,杨争,席冬冬,等.新乡市秋季大气细颗粒物PM2.5中水溶性离子特征及其来源解析[J].环境科学学报,2018,38(2):640-648.(In English:Yan GX,Yang Z,Xi DD,et al.Characterization and source analysis of the water-soluble inorganic ions in PM2.5 of Xinxiang during autumn[J].Acta Sci Circumstant,2018,38(2):640-648.)
[19] 邱婷,周家斌,肖经汗,等.武汉市秋、冬季大气PM2.5中水溶性离子污染特征及来源分析[J].环境污染与防治,2015,37(4):17-20.(In English:Qiu T,Zhou JB,Xiao JH,et al.Characteristics and sources apportionment of water-soluble ions in PM2.5 in autumn and winter of Wuhan[J].Environ Poll Control,2015,37(4):17-20.)
[20] 周登,张帆,吴涛涛,等.冬季霾天气下武汉城区大气PM2.5的化学特征[J].湖北农业科学,2014,53(21):5109-5111,5115.(In English:Zhou D,Zhang F,Wu TT,et al.Chemical characteristics of PM2.5 under winter haze days in urban Wuhan[J].Hubei Agric Sci,2014,53(21):5109-5111,5115.)
[21] 王明毅,吴洪波.武汉城区春节PM2.5中水溶性无机离子污染特征[J].环境科学与技术,2016,39(6):80-85.(In English:Wang MY,Wu HB.Characterization and source analysis of water-soluble inorganic ions in PM2.5 during spring festival in Wuhan[J].Environ Sci Technol,2016,39(6):80-85.)
[22] Fu XX,Guo H,Wang XM,et al.PM2.5 acidity at a background site in the Pearl River Delta region in fall-winter of 2007-2012[J].J Hazard Mater,2015,286:484-492.
[23] 赵普生,张小玲,孟伟,等.京津冀区域气溶胶中无机水溶性离子污染特征分析[J].环境科学,2011,32(6):1546-1549.(In English:Zhao PS,Zhang XL,Meng W,et al.Characteristics of inorganic water-soluble ions from aerosols in Beijing-Tianjin-Hebei Area[J].Chin J Environ Sci,2011,32(6):1546-1549.)
[24] 段凤魁,刘咸德,鲁毅强,等.北京市大气颗粒物的浓度水平和离子物种的化学形态[J].中国环境监测,2003,19(1):13-17.(In English:Duan FK,Liu XD,Lu YQ,et al.Concentration level of TSP and chemical speciation of ion species in Beijing[J].Environ Monitor China,2003,19(1):13-17.)
[25] 温天雪,王跃思,张凯.采暖季北京大气PM10中硫酸盐与硫氧化率的观测研究[J].中国科学院研究生院学报,2007,24(5):584-589.(In English:Wen TX,Wang YS,Zhang K.Study on sulfate and sulfur oxidation ratio in PM10 during heating season in Beijing[J].J Grad School Chin Acad Sci,2007,24(5):584-589.)
[26] 中华人民共和国国家质量监督检验检疫总局,中国国家标准化管理委员会.GB 3095—2012 环境空气质量标准[S].北京:中国环境科学出版社,2016.(In English:General Administration of Quality Supervision,Inspection and Quarantine of the People's Republic of China,National Standardization Management Committee of China.GB 3095-2012 Ambient air quality standard[S].Beijing:China Environmental Science Press,2016.)
[27] 孙韧,张文具,董海燕,等.天津市PM10和PM2.5中水溶性离子化学特征及来源分析[J].中国环境监测,2014,30(2):145-150.(In English:Sun R,Zhang WJ,Dong HY,et al.Chemical character and source analysis of water-soluble irons in PM10 and PM2.5 in Tianjin City[J].Environ Monitor China,2014,30(2):145-150.)
[28] Quan JN,Tie XX,Zhang Q,et al.Characteristics of heavy aerosol pollution during the 2012-2013 winter in Beijing,China[J].Atmos Environ,2014,88:83-89.
[29] Huang RJ,Zhang YL,Bozzetti C,et al.High secondary aerosol contribution to particulate pollution during haze events in China[J].Nature,2014,514(7521):218-222.
[30] Khoder MI.Atmospheric conversion of sulfur dioxide to particulate sulfate and nitrogen dioxide to particulate nitrate and gaseous nitric acid in an urban area[J].Chemosphere,2002,49(6):675-684.
[2] 薛元恺,周丽玲.我国灰霾天气成因与防治对策探讨[J].环境卫生学杂志,2017,7(3):248-254.(In English:Xue YK,Zhou LL.Causes and control measures of hazy weather in China[J].J Environ Hyg,2017,7(3):248-254.)
[3] Squizzato S,Masiol M,Brunelli A,et al.Factors determining the formation of secondary inorganic aerosol:a case study in the Po Valley (Italy)[J].Atmos Chem Phys,2013,13(4):1927-1939.
[4] Forster P,Ramaswamy V,Artaxo P,et al.Changes in atmospheric constituents and in radiative forcing[M]//Solomon S,Qin D,Manning M,et al.Climate Change 2007:The Physical Science Basis:Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change.New York:Cambridge University Press,2007.
[5] B?umer D,Vogel B,Versick S,et al.Relationship of visibility,aerosol optical thickness and aerosol size distribution in an ageing air mass over south -west Germany[J].Atmos Environ,2008,42(5):989-998.
[6] Novakov T,Penner JE.Large contribution of organic aerosols to cloud-condensation-nuclei concentrations[J].Nature,1993,365(6449):823-826.
[7] Haywood J,Bush M,Abel S,et al.Prediction of visibility and aerosol within the operational Met Office Unified Model.Ⅱ:validation of model performance using observational data[J].Quart J Roy Meteor Soc,2008,134(636):1817-1832.
[8] 刀谞,张霖琳,王超,等.京津冀冬季与夏季PM2.5/PM10及其水溶性离子组分区域性污染特征分析[J].环境化学,2015,34(1):60-69.(In English:Dao X,Zhang LL,Wang C,et al.Characteristics of mass and ionic compounds of atmospheric particles in winter and summer of Beijing-Tianjin-Hebei area,China[J].Environ Chem,2015,34(1):60-69.)
[9] 阴丽淑,李金娟,郭兴强,等.贵州“两控区”城市PM2.5及其阴阳离子污染特征[J].中国环境科学,2017,37(2):416-423.(In English:Yin LS,Li JJ,Guo XQ,et al.Pollution characteristics of concentrations and it's ions in PM2.5 of sulfur and acid-rain Control Zone Cities,Guizhou Province[J].China Environ Sci,2017,37(2):416-423.)
[10] 葛顺,汤莉莉,秦玮,等.南京地区秋季灰霾天气特征及其水溶性离子分析[J].环境科学与技术,2015,38(2):99-104.(In English:Ge S,Tang LL,Qin W,et al.Characteristics analysis of haze and water-soluble ion in Nanjing in Autumn[J].Environ Sci Technol,2015,38(2):99-104.)
[11] Long SL,Zeng JR,Li Y,et al.Characteristics of secondary inorganic aerosol and sulfate species in size -fractionated aerosol particles in Shanghai[J].J Environ Sci,2014,26(5):1040-1051.
[12] 孟晓艳,余予,张志富,等.2013年1月京津冀地区强雾霾频发成因初探[J].环境科学与技术,2014,37(1):190-194.(In English:Meng XY,Yu Y,Zhang ZF,et al.Preliminary study of the dense fog and haze events' formation over Beijing-Tianjin-and-Hebei region in January of 2013[J].Environ Sci Technol,2014,37(1):190-194.)
[13] Xu LL,Chen XQ,Chen JS,et al.Seasonal variations and chemical compositions of PM2.5 aerosol in the urban area of Fuzhou,China[J].Atmos Res,2012,104-105:264-272.
[14] 范美益,曹芳,张园园,等.徐州市冬季大气细颗粒物水溶性无机离子污染特征及来源解析[J].环境科学,2017,38(11):4478-4485.(In English:Fan MY,Cao F,Zhang YY,et al.Characteristics and sources of water soluble inorganic ions in fine particulate matter during winter in Xuzhou[J].Environ Sci,2017,38(11):4478-4485.)
[15] 王晓琦,周颖,程水源,等.典型城市冬季PM2.5水溶性离子污染特征与传输规律研究[J].中国环境科学,2016,36(8):2289-2296.(In English:Wang XQ,Zhou Y,Cheng SY,et al.Characterization and regional transmission impact of water-soluble ions in PM2.5 during winter in typical cities[J].China Environ Sci,2016,36(8):2289-2296.)
[16] 魏巧珍,王宇红,李盛,等.基于PCA-MLR模型的兰州市大气PM2.5污染来源解析[J].环境卫生学杂志,2017,7(4):267-273.(In English:Wei QZ,Wang YH,Li S,et al.The source apportionment of PM2.5 based on PCA-MLR model in Lanzhou City[J].J Environ Hyg,2017,7(4):267-273.)
[17] 幸娇萍,邵龙义,李红,等.北京灰霾天PM2.5中有机官能团和无机离子的ATR-FTIR研究[J].中国环境科学,2016,36(6):1654-1659.(In English:Xing JP,Shao LY,Li H,et al.ATR-FTIR characterization of organic functional groups and inorganic ions of the haze PM2.5 in Beijing[J].China Environ Sci,2016,36(6):1654-1659.)
[18] 闫广轩,杨争,席冬冬,等.新乡市秋季大气细颗粒物PM2.5中水溶性离子特征及其来源解析[J].环境科学学报,2018,38(2):640-648.(In English:Yan GX,Yang Z,Xi DD,et al.Characterization and source analysis of the water-soluble inorganic ions in PM2.5 of Xinxiang during autumn[J].Acta Sci Circumstant,2018,38(2):640-648.)
[19] 邱婷,周家斌,肖经汗,等.武汉市秋、冬季大气PM2.5中水溶性离子污染特征及来源分析[J].环境污染与防治,2015,37(4):17-20.(In English:Qiu T,Zhou JB,Xiao JH,et al.Characteristics and sources apportionment of water-soluble ions in PM2.5 in autumn and winter of Wuhan[J].Environ Poll Control,2015,37(4):17-20.)
[20] 周登,张帆,吴涛涛,等.冬季霾天气下武汉城区大气PM2.5的化学特征[J].湖北农业科学,2014,53(21):5109-5111,5115.(In English:Zhou D,Zhang F,Wu TT,et al.Chemical characteristics of PM2.5 under winter haze days in urban Wuhan[J].Hubei Agric Sci,2014,53(21):5109-5111,5115.)
[21] 王明毅,吴洪波.武汉城区春节PM2.5中水溶性无机离子污染特征[J].环境科学与技术,2016,39(6):80-85.(In English:Wang MY,Wu HB.Characterization and source analysis of water-soluble inorganic ions in PM2.5 during spring festival in Wuhan[J].Environ Sci Technol,2016,39(6):80-85.)
[22] Fu XX,Guo H,Wang XM,et al.PM2.5 acidity at a background site in the Pearl River Delta region in fall-winter of 2007-2012[J].J Hazard Mater,2015,286:484-492.
[23] 赵普生,张小玲,孟伟,等.京津冀区域气溶胶中无机水溶性离子污染特征分析[J].环境科学,2011,32(6):1546-1549.(In English:Zhao PS,Zhang XL,Meng W,et al.Characteristics of inorganic water-soluble ions from aerosols in Beijing-Tianjin-Hebei Area[J].Chin J Environ Sci,2011,32(6):1546-1549.)
[24] 段凤魁,刘咸德,鲁毅强,等.北京市大气颗粒物的浓度水平和离子物种的化学形态[J].中国环境监测,2003,19(1):13-17.(In English:Duan FK,Liu XD,Lu YQ,et al.Concentration level of TSP and chemical speciation of ion species in Beijing[J].Environ Monitor China,2003,19(1):13-17.)
[25] 温天雪,王跃思,张凯.采暖季北京大气PM10中硫酸盐与硫氧化率的观测研究[J].中国科学院研究生院学报,2007,24(5):584-589.(In English:Wen TX,Wang YS,Zhang K.Study on sulfate and sulfur oxidation ratio in PM10 during heating season in Beijing[J].J Grad School Chin Acad Sci,2007,24(5):584-589.)
[26] 中华人民共和国国家质量监督检验检疫总局,中国国家标准化管理委员会.GB 3095—2012 环境空气质量标准[S].北京:中国环境科学出版社,2016.(In English:General Administration of Quality Supervision,Inspection and Quarantine of the People's Republic of China,National Standardization Management Committee of China.GB 3095-2012 Ambient air quality standard[S].Beijing:China Environmental Science Press,2016.)
[27] 孙韧,张文具,董海燕,等.天津市PM10和PM2.5中水溶性离子化学特征及来源分析[J].中国环境监测,2014,30(2):145-150.(In English:Sun R,Zhang WJ,Dong HY,et al.Chemical character and source analysis of water-soluble irons in PM10 and PM2.5 in Tianjin City[J].Environ Monitor China,2014,30(2):145-150.)
[28] Quan JN,Tie XX,Zhang Q,et al.Characteristics of heavy aerosol pollution during the 2012-2013 winter in Beijing,China[J].Atmos Environ,2014,88:83-89.
[29] Huang RJ,Zhang YL,Bozzetti C,et al.High secondary aerosol contribution to particulate pollution during haze events in China[J].Nature,2014,514(7521):218-222.
[30] Khoder MI.Atmospheric conversion of sulfur dioxide to particulate sulfate and nitrogen dioxide to particulate nitrate and gaseous nitric acid in an urban area[J].Chemosphere,2002,49(6):675-684.