重庆市不同粒径颗粒物中水溶性离子污染特征

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Abstract PM_1.0, PM_2.5 and PM₁₀ samples were collected from March 2010 to February 2011 and January 2017 to December 2017 in the urban area of Chongqing. The mass concentrations of nine water-soluble inorganic ions (WSIIs) were determined by anion chromatography, and characteristics of WSIIs inmulti-size particles during recent years were investigated. The results showed that the annualmean concentrationsof WSIIs in PM_1.0, PM_1.0~2.5 and PM_2.5~10 were 24.10, 32.89 and 39.11μg/m³ respectively, accounting for 41.8%, 40.3% and 38.6% of PM respectively in 2017. The annual mean concentrations of WSIIs in PM in 2010 (39.85, 47.84 and 57.12μg/m³ respectively) were higher than that in 2017, and so were thefractions (49.2%, 46.6% and 36.2% respectively). However, the concentrations and fractions of NO₃^- in PM increased by 12.3%~27.8% and 53.1%~8.2% respectively from 2010 to 2017, and NO₃^- was the primary ion in 2017 winter. SO₄^2-, NO₃^-, NH₄⁺, Cl^-, K⁺, and Na⁺ were mainly distributed in fine particles, while F^-, Mg²⁺ and Ca²⁺ were the major WSIIs components in coarse particles. The particles in Chongqing were slightly alkaline, especially coarse particles, and NH₄⁺ were existed in the form of (NH₄)₂SO₄ and NH₄NO₃. Compared with that in 2010, the concentrations of both SO₄^2- and NO₃^- increased with the increase of relative humidity in fine particles in 2017. RH-dependent heterogeneous reactions contributed greatly to the formation of sulfate and nitrate in 2017, especially in PM_1.0. With the aggravation of pollution, the evolution processes of different ions were differentinmulti-size particles. Among them, the concentrations and fractions of NO₃^- in WSIIs increased significantly and NO₃^- was the primarily driver of heavy pollution in fine particles in 2017, while the contributions of SO₄^2- and the ions from dust (Mg²⁺ and Ca²⁺) decreased. In addition, themass ratios of NO₃^-/SO₄^2- in different particle size increased with the aggravation of pollution and were higher than 1.0 during the heavy pollution days in 2017, but not in 2010. The main sources of WSIIs in fine particles were secondary formation, while dust was the major source of WSIIs incoarse particles. The pollution of dust in 2017 was lighter than that in 2010, but the contribution of secondary formation was increased significantly from 2010 to 2017, especially the formation of nitrate in Chongqing. The control of NO_x emission sourcesis critical to reduce WSIIs emission. Results provided important information for the study of the sources and formation mechanisms of the atmospheric particles in Chongqing.

Key words： water-soluble inorganic ions size distribution seasonal variation evolution processes Chongqing

Received: 20 February 2021

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X513

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	PENG Chao
	ZHANG Dan
	FANG Wei-kai
	WANG Xiao-chen
	XIE Geng
	XIANG Ying
	LI Zhen-liang

Cite this article:

PENG Chao,ZHANG Dan,FANG Wei-kai等. Characteristics ofwater-solubleionsinmulti-sizeparticlesin Chongqing[J]. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(10): 4529-4540.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2021/V41/I10/4529

[1]	Tian S L, Pan Y P, Wang Y S. Ion balance and acidity of size-segregated particles during haze episodes in urban Beijing[J]. Atmospheric Research, 2018,201:159-167.
[2]	Zhang YL, Cao F. Fine particulatematter (PM2.5) in China at a city level[J]. Scientific Reports, 2015,5:14884-14895.
[3]	孙有昌,姜楠,王申博,等.安阳市大气PM2.5中水溶性离子季节特征及来源解析[J]. 环境科学, 2020,41(1):75-81.Sun Y C, Jiang N, Wang S B, et al. Seasonal characteristics and source analysis of water-soluble ions in PM2.5 of Anyang city[J]. Environmental Science, 2020,41(1):75-81.
[4]	WangL, Ji D, Li Y, et al. The impact of relative humidity on the size distribution and chemical processes ofmajor water-soluble inorganic ions in themegacity of Chongqing, China[J]. Atmospheric Research, 2017,192:19-29.
[5]	Intergovernmental Panel on Climate Change (IPCC). Fifth Assessment Report[R]. Cambridge University Press, Cambridge. 2014.
[6]	Guo S, Hu M, Zamora M L, et al. Elucidating severe urban haze formation in China[J]. Proceedings of the National Academy of Sciences of the United States of America, 2014,111(49):17373-17378.
[7]	Sun YL, Wang Z F, Fu P Q, et al. Aerosol composition, sources and processes during wintertime in Beijing, China[J]. Atmospheric Chemistry and Physics, 2013,13(9):4577-4592.
[8]	Francisco SS, Rovira J, Mari M, et al. Main components and human health risks assessment of PM10, PM2.5, and PM1 in two areas influenced by cement plants[J]. Atmospheric Environment, 2015,120:109-116.
[9]	Liu M X, Song Y, Zhou T, et al. Fine particle pH during severe haze episodes in northern China[J]. Geophysical Research Letters, 2017, 44(10):5213-5221.
[10]	Seinfeld J H, Pandis S N. From air pollution to climate change[M]. New Jersey:John Wiley & Sons, Inc., 2016:423-439.
[11]	Zhuang H, Chan C K, Fan M, et al. Formation of nitrate and non-sea-salt sulfate on coarse particles[J]. Atmospheric Environment, 1999,33:4223-4233.
[12]	李彦沛,郝庆菊,温天雪,等.重庆市北碚城区气溶胶中水溶性无机离子的质量浓度及其粒径分布[J]. 环境科学, 2018,39(9):4002-4013.Li Y P, Hao Q J, Wen T X, et al. Mass concentrations and size distributions of water-soluble inorganic ions in atmospheric aerosols in Beibei district, Chongqing[J]. Environmental Science, 2018,39(9):4002-4013.
[13]	陶月乐,李亲凯,张俊,等.成都市大气颗粒物粒径分布及水溶性离子组成的季节变化特征[J]. 环境科学, 2017,38(10):4034-4043.Tao Y L, Li Q K, Zhang J, et al. Seasonal variations in particle size distribution and water-soluble ion composition of atmospheric particles in Chengdu[J]. Environmental Science, 2017,38(10):4034-4043.
[14]	Yao X H, Lau A P S, Fang M, et al. Size distributions and formation of ionic species in atmospheric particulate pollutants in Beijing, China:1-inorganic ions[J]. Atmospheric Environment, 2003,37(21):2991-3000.
[15]	耿彦红,刘卫,单健,等.上海市大气颗粒物中水溶性离子的粒径分布特征[J]. 中国环境科学, 2010,30(12):1585-1589.Geng Y H, Liu W, Shan J, et al. Characterization of major water-soluble ions in size-fractionated particulate matters in Shanghai[J]. China Environmental Science, 2010,30(12):1585-1589.
[16]	Liu Z R, Xie Y Z, Hu B, et al. Size-resolved aerosol water-soluble ions during the summer and winter seasons in Beijing:Formationmechanisms of secondary inorganic aerosols[J]. Chemosphere, 2017,183:119-131.
[17]	Shao P Y, Tian H Z, Sun Y J, et al. Characterizing remarkable changes of severe haze events and chemical compositions inmulti-size airborne particles (PM1, PM2.5 and PM10) from January 2013 to 2016~2017 winter in Beijing, China[J]. Atmospheric Environment, 2018,189:133-144.
[18]	He K B, Zhao Q, Ma Y L, et al. Spatial and seasonal variability of PM2.5 acidity at two Chinesemegacities:insights into the formation of secondary inorganic aerosols[J]. Atmospheric Chemistry and Physics, 2012,12(3):1377-1395.
[19]	Sun Y L, Jiang Q, Wang Z F, et al. Investigation of the sources and evolution processes of severe haze pollution in Beijing in January 2013[J]. Journal of Geophysical Research:Atmospheres, 2014,119:4380-4398.
[20]	Tian SL, Pan Y P, Wang Y S. Size-resolved source apportionment of particulatematter in urban Beijing during haze and non-haze episodes[J]. Atmospheric Chemistry and Physics, 2016,16(1):1-19.
[21]	Gao Y, Lee S C, Huang Y, et al. Chemical characterization and source apportionment of size-resolved particles in Hongkong sub-urban area[J]. Atmospheric Research, 2016,170:112-122.
[22]	Wang H B, Tian M, Chen Y, et al. Seasonal characteristics, formationmechanisms and source origins of PM2.5 in twomegacities in Sichuan Basin, China[J]. Atmospheric Chemistry and Physics, 2018, 18(2):865-881.
[23]	Tian M, Liu Y, Yang F M, et al. Increasing importance of nitrate formation for heavy aerosol pollution in twomegacities in Sichuan Basin, southwest China[J]. Environmental Pollution, 2019,250:898-905.
[24]	Tian M, Wang H B, Chen Y, et al. Highly time-resolved characterization of water-soluble inorganic ions in PM2.5 in a humid and acidicmegacity in Sichuan Basin, China[J]. Science of the Total Environment, 2017,580:224-234.
[25]	Qiao B Q, Chen Y, Tian M, et al. Characterization of water soluble inorganic ions and their evolution processes during PM2.5 pollution episodes in a small city in southwest China[J]. Science of the Total Environment, 2019,650:2605-2613.
[26]	李欢,唐贵谦,张军科,等.2017~2018年北京大气PM2.5中水溶性无机离子特征[J]. 环境科学, 2020,41(10):4364-4373.Li H, Tang G Q, Zhang J K. Characteristics of water-soluble inorganic ions in PM2.5 in Beijing during 2017~2018[J]. Environmental Science, 2020,41(10):4364-4373.
[27]	张懿华,王东方,赵倩彪,等.上海城区PM2.5中有机碳和元素碳变化特征及来源分析[J]. 环境科学, 2014,35(9):3263-3270.Zhang Y H, Wang D F, Zhao Q B, et al. Characteristics and sources of organic carbon and elemental carbon in PM2.5 in Shanghai urban area[J]. Environmental Science, 2014,35(9):3263-3270.
[28]	朱倩茹,刘永红,徐伟嘉,等.广州PM2.5污染特征及影响因素分析[J]. 中国环境监测, 2013,29(2):15-21.Zhu Q R, Liu Y H, Xu W J, et al. Analysis on the pollution characteristics and influence factors of PM2.5 in Guangzhou[J]. Environmental Monitoring in China, 2013,29(2):15-21.
[29]	程渊,吴建会,毕晓辉,等.武汉市大气PM2.5中水溶性离子污染特征及来源[J]. 环境科学学报, 2019,39(1):189-196.Cheng Y, Wu J H, Bi X H, et al. Characteristics and source apportionment of water-soluble ions in ambient PM2.5 in Wuhan,China[J]. Acta Scientiae Circumstantiae, 2019,39(1):189-196.
[30]	杜翔,赵普生,苏捷,等.北京地区气溶胶水溶性组分粒径分布特征[J]. 环境科学, 2018,39(1):4858-4865.Du X, Zhao P S, Su J, et al. Size distributions of water-soluble components in ambient aerosol of Beijing[J]. Environmental Science, 2018,39(1):4858-4865.
[31]	王佳,李晓,吴瑞杰,等.郑州市PM2.5和PM10中水溶性无机离子的污染特征[J]. 郑州大学学报(理学版), 2014,46(4):81-87.Wang J, Li X, Wu R J, et al. Pollution characteristics of water-soluble ions in PM2.5 and PM10 in Zhengzhou[J]. Journal of Zhengzhou University (Natural Science Ed.), 2014,46(4):81-87.
[32]	张胜华,黄伊宁,毛文文,等.上海大气颗粒物中无机离子的粒径分布及其季节变化[J]. 环境科学学报, 2019,39(1):72-79.Zhang S H, Huang Y N, Mao W W, et al. Seasonal variations of the size distributions of inorganic ions in the atmospheric particles in Shanghai[J]. Acta Scientiae Circumstantiae, 2019,39(1):72-79.
[33]	Yang Y J, Zhou R, Yu Y, et al. Size-resolved aerosol water-soluble ions at a regional background station of Beijing, Tianjin, and Hebei, North China[J]. Journal of Environmental Sciences, 2017,55:146-156.
[34]	Huang X J,Liu Z R, Zhang J K, et al. Seasonal variation and secondary formation of size-segregated aerosol water-soluble inorganic ions during pollution episodes in Beijing[J]. Atmospheric Research, 2016, 168:70-79.
[35]	Yang Y J, Zhou R, Wu J J, et al. Seasonal variations and size distributions of water-soluble ions in atmospheric aerosols in Beijing, 2012[J]. Journal of Environmental Sciences, 2015,34:197-205.
[36]	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.Duan F K, Liu X D, Lu Y Q, et al. Concentrat ion level of TSP and chemical speciation of ion species in Beijing[J]. Environmental Monitoring in China, 2003,19(1):13-17.
[37]	Yao X H, 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.
[38]	XuL L, Duan F K, He K B, et al. Characteristics of the secondary water-soluble ions in a typical autumn haze in Beijing[J]. Environmental Pollution, 2017,227:296-305.
[39]	刘臻,祁建华,王琳,等.青岛大气气溶胶水溶性无机离子的粒径分布特征[J]. 中国环境科学, 2012,32(8):1422-1432.Liu Z, Qi J H, Wang L, et al. Particle size distribution of water-soluble inorganic ions of atmospheric aerosol in Qingdao[J]. China Environmental Science, 2012,32(8):1422-1432.
[40]	Wei N N, Xu Z Y, Liu J W, et al. Characteristics of size distributions and sources of water-soluble ions in Lhasa duringmonsoon and non-monsoon seasons[J]. Journal of Environmental Sciences, 2019, 82:155-168.
[41]	Peng C, Tian M, Chen Y, et al. Characteristics, formation mechanisms and potential transport pathways of PM2.5 at a rural background site in Chongqing, Southwest China[J]. Aerosol and Air Quality Research, 2019,19(9):1980-1992.
[42]	张丹,翟崇治,周志恩,等.重庆市主城区不同粒径颗粒物水溶性无机组分特征[J]. 环境科学研究, 2012,25(10):1099-1106.Zhang D, Zhai C Z, Zhou Z E, et al. Characteristics of water-soluble inorganic ions in different size particles in Chongqing[J]. Research of Environmental Sciences, 2012,25(10):1099-1106.
[43]	Cheng C L, Wang G H, Meng J J, et al. Size-resolved airborne particulate oxalic and related secondary organic aerosol species in the urban atmosphere of Chengdu, China[J]. Atmospheric Research, 2015,161-162:134-142.
[44]	Deshmukh D K, Kawamura K, Debm K. Dicarboxylic acids, ω-oxocarboxylic acids, α-dicarbonyls, WSOC, OC, EC, and inorganic ions in wintertime size-segregated aerosols from central India:Sources and formation processes[J]. Chemosphere, 2016,161:27-42.
[45]	Ge X L, Zhang Q, Sun Y L, et al. Effect of aqueous-phase processing on aerosol chemistry and size distributions in Fresno, California, during wintertime[J]. Environmental Chemistry, 2012,9(3):221-235.
[46]	Zhang G H, Bi X H, ChanL Y, et al. Enhanced trimethylamine-containing particles during fog events detected by single particle aerosolmass spectrometry in urban Guangzhou, China[J]. Atmospheric Environment, 2012,55:121-126.
[47]	张灿,周志恩,翟崇治,等.重庆市主城区NH3排放估算及分布特征分析[J]. 环境污染与防治, 2013,35(10):65-70.Zhang C, Zhou Z E, Zhai C Z, et al. Estimate and distribution analyze of NH3emission in Chongqing urban city[J]. Environmental Pollution & Control, 2013,35(10):65-70.
[48]	张六一.三峡库区大气氮沉降特征、通量及其对水体氮素的贡献[D]. 北京:中国科学院大学, 2019.Zhang L Y. Atmospheric nitrogen deposition in the Three Gorges Reservoir area:characteristics, fluxes, and contributions to the aquatic environment[D]. Peking:University of Chinese Academy of Sciences, 2019.
[49]	Chen Y, Tian M, Huang R J, et al. Characterization of urban amine-containing particles in southwestern China:Seasonal variation, source, and processing[J]. Atmospheric Chemistry and Physics, 2019,19(5):3245-3255.
[50]	Zhao X Y, Wang X M, Ding X, et al. Compositions and sources of organic acids in fine particles (PM2.5) over the Pearl River Delta region, south China[J]. Journal of Environmental Sciences, 2014,26(1):110-121.
[51]	闫广轩,张靖雯,雷豪杰,等.郑州市大气细颗粒物中水溶性离子季节性变化特征及其源解析[J]. 环境科学, 2019,40(4):1545-1552.Yan G X, Zhang J W, Lei H J, et al. Seasonal variation and source analysis of water-soluble inorganic ions in fine particulate matter in Zhengzhou[J]. Environmental Science, 2019,40(4):1545-1552.
[52]	Li H M, Wang Q Q, Yang M, et al. Chemical characterization and source apportionment of PM2.5 aerosols in amegacity of Southeast China[J]. Atmospheric Research, 2016,181:288-299.
[53]	Fan J W, Zhang R Y, Collins D, et al. Contribution of secondary condensable organics to new particle formation:A case study in Houston, Texas[J]. Geophysical ResearchLetters, 2006,33:1-4.
[54]	Zhou H J, Lü C W, He J, et al. Stoichiometry of water-soluble ions in PM2.5:Application in source apportionment for a typical industrial city in semi-arid region, Northwest China[J]. Atmospheric Research, 2018,204:149-160.
[55]	Wang Y, Zhuang G S, Tang A, et al. The evolution of chemical components of aerosols at fivemonitoring sites of China during dust storms[J]. Atmospheric Environment, 2007,41(5):1091-1106.
[56]	Rastogi N, Sarinm M. Chemistry of aerosols over a semi-arid region:Evidence for acid neutralization bymineral dust[J]. Geophysical ResearchLetters, 2006,33:1-4.
[57]	Tian Y Z, Wu J H, Shi G L, et al.Long-term variation of the levels, compositions and sources of size-resolved particulatematter in amegacity in China[J]. Science of The Total Environment, 2013, 463-464:462-468.
[58]	Deng XL, Shi C E, Wu B W, et al. Characteristics of the water-soluble components of aerosol particles in Hefei, China[J]. Journal of Environmental Sciences, 2016,42:32-40.
[59]	Meng C C, WangL T, Zhang F F, et al. Characteristics of concentrations and water-soluble inorganic ions in PM2.5 in Handan City, Hebei province, China[J]. Atmospheric Research, 2016,171:133-146.
[60]	HJ 633-2012环境空气质量指数技术规定[S].HJ 633-2012 Technical regulation on ambient air quality indes[S].