Abstract:In order to understand the characteristics of water-soluble ion pollution of atmospheric fine particles in the urban area of Chengdu, a total of 102 PM2.5 samples were collected in the urban areas of Chengdu in four seasons. Mass concentrations of particles matter (PM) and its water-soluble ions (NH4+、Ca2+、Na+、Mg2+、K+、F-、NO3-、SO42-、Cl-) were measured and analyzed to characterize its seasonal, with special attentions to characteristics and formation of secondary ions. The results showed that concentration changes of water-soluble ions and atmospheric fine particles in Chengdu’s urban area generally followed the same pattern. Secondary inorganic ions (NH4+、NO3-、SO42-) were the main components of water-soluble ions in PM, accounting for 84.8%. Atmospheric fine particles appeared to be acidic in Spring, Autumn, and Winter, and their in-situ PH values were 1.9, 2.6 and 2.0, respectively. Sulfate and nitrate in the atmospheric PM exhibited differences in its chemical characteristics. For example, the dominating form of sulfate was NH4HSO4, which mainly resulted from heterogeneous reaction processes and was heavily affected by the regional atmospheric transportation; while the dominating form of nitrate was NH4NO3, which mainly resulted from homogeneous reaction processed and was heavily affected by local emissions.
Baccarelli A A, Zheng Y, Zhang X, et al. Air pollution exposure and lung function in highly exposed subjects in Beijing, China:a repeated-measure study[J]. Particle & Fibre Toxicology, 2014,11(1):51.
[2]
韦莲芳,杨复沫,谭吉华,等. 大气气溶胶消光性质的研究进展[J]. 环境化学, 2014,33(5):705-715. Wei L F, Yang F M, Tan J H, et al. Research progress on aerosol extinction properties[J]. Environmental Chemistry, 2014,33(5):705-715.
[3]
Zhang H Y, Cheng S Y, Li J B, et al. Investigating the aerosol mass and chemical components characteristics and feedback effects on the meteorological factors in the Beijing-Tianjin-Hebei region, China.[J]. Environmental Pollution, 2019,244:495-502.
[4]
吴兑,廖碧婷,陈慧忠,等.珠江三角洲地区的灰霾天气研究进展[J]. 气候与环境研究, 2014,19(2):248-264. Wu D, Liao B T, Chen H Z, et al. Advances in studies of haze weather over Pearl River Delta. Climatic and Environmental Research, 2014,19(2):248-264.
[5]
何沐全,刘志红,张颖,等.川南城市群大气灰霾时空分布特征及成因分析[J]. 中国环境科学, 2017,37(2):432-442. He M Q, Liu Z H, Zhang Y, et al. Analyses on the spatial-temporal distribution features and causing factors of atmospheric haze in the southern city-group of Sichuan[J]. China Environmental Science, 2017,37(2):432-442.
[6]
黄丹丹.上海城区二次污染物形成过程及影响因素研究[J]. 环境科学学报, 38(6):2262-2269. Huang D D. Formation of secondary species in submicron particulate matter(PM1)in downtown Shanghai-episodic analysis[J]. Acta Scientiae Circumstantiae, 38(6):2262-2269.
[7]
Zhou J B, Xing Z Y, Deng J J, et al. Characterizing and sourcing ambient PM2.5 over key emission regions in China I:Water-soluble ions and carbonaceous fractions[J]. Atmospheric Environment, 2016, 135:20-30.
[8]
Mo H Q, Li L, Lai W, et al. Characterization of summer PM2.5 aerosols from four forest areas in Sichuan, SW China[J]. Particuology, 2015,20(3):94-103.
[9]
Andreae M O, Schmid O, Yang H, et al. Optical properties and chemical composition of the atmospheric aerosol in urban Guangzhou, China[J]. Atmospheric Environment, 2008,42(25):6335-6350.
[10]
张蒙,韩力慧,刘保献,等.北京市冬季重污染期间PM2.5及其组分演变特征[J]. 中国环境科学, 2020,40(7):2829-2838. Zhang M, Han L H, Liu B X, et al. Evolution of PM2.5 and its components during heavy pollution episodes in winter in Beijing[J]. China Environmental Science, 2020,40(7):2829-2838.
[11]
Haeng B B, P A V, Quansong T. Chemical coupling between ammonia, acid gases, and fine particles[J]. Environmental Pollution, 2004,129(1):89-98.
[12]
黄丹丹,周敏,余传冠,等.长三角淳安地区二次颗粒物污染形成机制[J]. 环境科学, 2018,39(12):5308-5314. Huang D D, Zhou M, Yu C G, et al. Physiochemical properties of the aerosol particles and their impacts on secondary aerosol formation at the background site of the Yangtze River Delta[J]. Environmental Science, 2018,39(12):5308-5314.
[13]
丁新航,梁越,肖化云,等.太原市采暖季清洁天与灰霾天PM2.5中水溶性无机离子组成及来源分析[J]. 环境化学, 2019,38(6):1356-1366. Ding X H, Liang Y, Xiao H Y, et al. Composition and source analysis of water-soluble inorganic ions of PM2.5 in clean and haze days during heating season in Taiyuan City[J]. Environmental Chemistry, 2019,38(6):1356-1366.
[14]
Liu M, 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.
[15]
Song S, Gao M, Xu W, et al. Fine-particle pH for Beijing winter haze as inferred from different thermodynamic equilibrium models[J]. Atmospheric Chemistry and Physics, 2018,18(10):7423-7438.
[16]
蒋琳,朱彬,王红磊,等.霾与轻雾天气下水溶性离子的组分特征-冬季长江三角洲地区一次污染过程分析[J]. 中国环境科学, 2017,37(10):3601-3610. Jiang L, Zhu B, Wang H L, et al. Characteristics of water-soluble ions in the haze and mist days in winter in Yangtze River Delta[J]. China Environmental Science, 2017,37(10):3601-3610.
[17]
Cheng S H, Yang L X, Zhou X H, et al. Size-fractionated water-soluble ions, situ pH and water content in aerosol on hazy days and the influences on visibility impairment in Jinan, China[J]. Atmospheric Environment, 2011,45(27):4631-4640.
[18]
付晓辛.珠江三角洲地区PM2.5浓度组成变化及其对粒子酸度和消光的影响[D]. 广州:中国科学院大学(广州地球化学研究所), 2015. Fu X X. Influence of PM2.5 major components on aerosol acidity and light extinction in the Pearl River Delta region[D]. Guangzhou:University of Chinese Academy of Sciences, 2015.
[19]
蒋琳.长三角颗粒物组分的理化特征及其对大气消光的影响[D]. 南京:南京信息工程大学, 2018. Jiang L. Physicochemical characteristics of aerosol components and their effects on atmospheric extinction in the Yangtze River Delta of China[D]. Nanjing:Nanjing University of Information Science & Technology, 2018.
[20]
Pathak R K, Yao X, Lau A K H, et al. Acidity and concentrations of ionic species of PM2.5 in Hong Kong[J]. Atmospheric Environment, 2003,37(8):1113-1124.
[21]
冯加良,胡小玲,管晶晶,等.上海市大气细颗粒物的酸度及其与组成的关系[J]. 上海大学学报(自然科学版), 2010,16(5):541-546. Feng J L, Hu X L, Guan J J, et al. Acidity of PM2.5 in Shanghai and its correlation with chemical composition of the particles[J]. Journal of Shanghai University (Natural Science), 2010,16(5):541-546.
[22]
何俊杰,吴耕晨,张国华,等.广州雾霾期间气溶胶水溶性离子的日变化特征及形成机制[J]. 中国环境科学, 2014,34(5):1107-1112. He J J, Wu G C, Zhang G H, et al. Diurnal variations and formation mechanisms of water-soluble inorganic ions in aerosols during a haze-fog period in Ghuangzhou[J]. China Environmental Science, 2014,34(5):1107-1112.
[23]
Pathak R K, Wu W S, Wang T. Summertime PM2.5 ionic species in four major cities of China:nitrate formation in an ammonia-deficient atmosphere[J]. Atmospheric Chemistry and Physics, 2009,9:1711-1722.
[24]
HJ 799-2016环境空气颗粒物水溶性阴离子的测定离子色谱法技术规范[S].
[25]
HJ 800-2016颗粒物水溶性阳离子的测定离子色谱法技术规范[S].
[26]
王振彬,刘安康,卢文,等.霾不同发展阶段下污染气体和水溶性离子变化特征分析[J]. 环境科学, 2019,40(12):5213-5223. Wang Z B, Liu A K, Lu W, et al. Change characteristics of pollution gas and water-soluble ions in different development stages of haze[J]. Environmental Science, 2019,40(12):5213-5223.
[27]
Wexler A S. Thermodynamic Model of the System H+-NH4+- SO42--NO3--H2O at Tropospheric Temperatures[J]. Journal of Physical Chemistry A, 1998,102(12):2137-2154.
[28]
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]. Atmospheric Chemistry and Physics, 2013,13:1927-1939.
[29]
Zhang Q, Jimenez J L, Worsnop D R, et al. A case study of urban particle acidity and its influence on secondary organic aerosol[J]. Environmental science & technology, 2007,41(9):3213-3219.
[30]
Ansari A S, Pandis S N. Response of inorganic PM to precursor concentrations[J]. Environmental Science & Technology, 1998,32:2706-2714.
[31]
杨溢巍.基于高时间分辨率观测的PM2.5粒子酸性特征研究[D]. 上海:复旦大学, 2014. Yang Y W. Study on the characteristics of PM2.5 acidity based on the high temporal resolution observations[D]. Shanghai:Fudan University, 2014.
[32]
HE K, ZHAO Q, MA Y, et al. Spatial and seasonal variability of PM2.5 acidity at two Chinese megacities:insights into the formation of secondary inorganic aerosols[J]. Atmospheric Chemistry and Physics, 2012,12:1377-1395.
[33]
赵晴.典型地区无机细粒子污染特征及成因研究[D]. 北京:清华大学, 2010. Zhao Q. Characteristics and formation of inorganic fine particluate pollution in typical regions of China[D]. Beijing:Tsinghua University, 2010.
[34]
Lin J J. Characterization of water-soluble ion species in urban ambient particles[J]. Environment International, 2002,28(1):55-61.
[35]
李欣悦,张凯山.成都市气态污染物NO2、SO2与大气颗粒物相关性分析[J]. 环境工程, 2019,37(6):111-116. Li X Y, Zhang K S. Analysis on relationships of gaseous pollutions NO2 and SO2 with atmospheric particles in Chengdu[J]. Environmental Engineering, 2019,37(6):111-116.
[36]
Zhao Q, He K, Rahn K A, et al. Dust storms come to Central and Southwestern China, too:implications from a major dust event in Chongqing[J]. Atmospheric Chemistry and Physics, 2010,10(6):2615-2630.
[37]
Pant P, Harrison R M. Estimation of the contribution of road traffic emissions to particulate matter concentrations from field measurements:A review[J]. Atmospheric Environment, 2013,77(7):78-97.
[38]
张晓雨.中国中东部地区典型城市大气细颗粒物中化学组成特征及来源解析研究[D]. 南京:南京大学, 2017. Zhang X Y. Study on chemical characteristics and source apportionments of fine particulates in the typical cities over the central and Eastern China[D]. Nanjing:Nanjing University, 2017.
[39]
代志光,张承中,李勇,等.西安夏季PM2.5中碳组分与水溶性无机离子特征分析[J]. 环境工程学报, 2014,8(10):4366-4372. Dai Z G, Zhang C Z, LI Y, et al. Analysis of carbon components and water-soluble inorganic ions in PM2.5 of Xi'an an during summer[J]. Chinese Journal of Environmental Engineering, 2014,8(10):4366-4372.
[40]
Hua Y, Cheng Z, Wang S X, et al. Characteristics and source apportionment of PM2.5 during a fall heavy haze episode in the Yangtze River Delta of China[J]. Atmospheric Environment, 2015, 123:380-391.
[41]
Liu L J S, Burton R, Wilson W E, et al. Comparison of aerosol acidity in urban and semi-rural environments[J]. Atmospheric Environment, 1996,30(8):1237-1245.
[42]
Bian Y X, Zhao C S, Ma N, et al. A study of aerosol liquid water content based on hygroscopicity measurements at high relative humidity in the North China Plain[J]. Atmospheric Chemistry and Physics, 2014,14(12):6417-6426.
[43]
Xue J, Lau A K H, Yu J Z. A study of acidity on PM2.5 in Hong Kong using online ionic chemical composition measurements[J]. Atmospheric Environment, 2011,45(39):7081-7088.
[44]
黄雄飞.广州城区气溶胶水溶性离子、酸性特征及其对采样误差的影响[D]. 广州:中山大学, 2009. Huang X F. Characteristics of water soluble ions and acidity of aerosol and the effect to sampling artifacts in urban Guangzhou[D]. Guangzhou:Sun Yat-Sen University, 2009.
[45]
Zhou Y, Xue L K, Wang T, et al. Characterization of aerosol acidity at a high mountain site in central eastern China[J]. Atmospheric Environment, 2012,51:11-20.
[46]
Song M D, Liu X, Tan Q W, et al. Characteristics and formation mechanism of persistent extreme haze pollution events in Chengdu, southwestern China[J]. Environmental Pollution, 2019,251:1-12.
[47]
李友平,周洪,张智胜,等.成都市城区PM2.5中二次水溶性无机离子污染特征[J]. 环境科学, 2014,35(12):4439-4445. Li Y P, Zhou H, Zhang S Z, et al. Pollution characteristics of secondary water-soluble inorganic ions of PM2.5 in urban Chengdu, China[J]. Environmental Science, 2014,35(12):4439-4445.
[48]
蒋燕,贺光艳,罗彬,等.成都平原大气颗粒物中无机水溶性离子污染特征[J]. 环境科学, 2016,37(8):2863-2870. Jiang Y, He G Y, Luo B, et al. Pollution characteristics of in atmospheric particulate matter in Chengdu plain[J]. Environmental Science, 2016,37(8):2863-2870.
[49]
Meng C C, Wang L 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.
[50]
杨复沫,贺克斌,马永亮,等.北京大气细粒子PM2.5的化学组成[J]. 清华大学学报(自然科学版), 2002,12:1605-1608. Yang F M, He K B, Ma Y L, et al. Chemical characteristics of PM2.5 species in Beijing ambient air[J]. Journal of Tsinghua University (Science and Technology), 2002,12:1605-1608.