深圳市冬季大气中硝酸分配特征观测研究

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摘要总硝酸(TNO₃=HNO₃+NO₃^-)的颗粒相分数ε(NO₃^-)决定了TNO₃在大气中的寿命,然而在冬季城市地区对该分配过程仍然掌握较少.本研究于2022年1月1日~1月31日分别在深圳市城区点位和路边点位对大气HNO₃、NO₃^-和相关污染物进行了在线连续观测.结果显示,深圳市城区冬季PM_2.5中NO₃^-的平均浓度为(6.3±3.9)μg/m³,占PM_2.5质量浓度的24.7%,是PM_2.5中最重要的成分之一.本次观测期间城区点位和路边点位ε(NO₃^-)均值分别为(0.81±0.13)和(0.75±0.16),TNO₃以向颗粒态分配为主.ε(NO₃^-)日变化特征均表现为白天相对较低,夜间较高,较高的温度、较低的湿度和较酸性的环境会增强硝酸盐的挥发并向气相分配,从而驱动ε(NO₃^-)的日变化.此外,气溶胶液态水含量(ALWC)和气溶胶pH值是影响深圳市冬季两个点位ε(NO₃^-)差异性的最重要因素,平均贡献率分别为41%和31%,在对大气硝酸的生成转化进行模式模拟时这两个因素需被重点考虑.

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	罗遥
	林晓玉
	牛英博
	云龙
	古添发
	林楚雄
	黄晓锋
	何凌燕

关键词 ：硝酸, 硝酸盐, 气溶胶pH值, 气溶胶液态水含量, 气粒分配

Abstract：The particle phase fraction of total nitrate determines its lifetime in the atmosphere, but this distribution process in urban areas in winter remain poorly understood. In this study, concentrations of HNO₃, NO₃^- and related pollutants was online observed at two sites (urban site and roadside site) in Shenzhen from January 1to January 31, 2022. During the observation period, the average concentration of NO₃^- was (6.3±3.9) μg/m³, accounting for 24.7% of the mass concentration of PM_2.5, which is one of the most important components of PM_2.5 in winter in Shenzhen. The mean values of ε(NO₃^-) at two sites were (0.81±0.13) and (0.75±0.16), respectively, and the distribution of nitrate was mainly to the particle phase. ε(NO₃^-) reflected the gas-particle partitioning of nitrate, and it was higher during nighttime and lower during daytime. The higher temperature, lower humidity and more acidic environment would enhance nitrate volatilization and its partitioning to gas phase, thus driving the diurnal variation of ε(NO₃^-). In addition, aerosol liquid water content and aerosol pH were the most important factors affecting the difference of two-site ε(NO₃^-) in winter of Shenzhen, with average contribution of 41% and 31%, respectively, indicating that these two factors should be taken into consideration when modeling the formation and transformation of gaseous nitric acid.

Key words： nitric acid nitrate aerosol pH aerosol liquid water content gas-particle partitioning

收稿日期: 2023-01-05

PACS:

X513

基金资助:深圳市科技计划项目(GXWD20201231165807007- 20200808165742001)

通讯作者: 何凌燕,教授,hely@pku.edu.cn E-mail: hely@pku.edu.cn

作者简介: 罗遥(1998-),男,湖北荆州人,硕士研究生,主要从事大气气溶胶中水溶性无机离子的研究.发表论文7篇.948974278@qq.com

引用本文:

罗遥, 林晓玉, 牛英博, 云龙, 古添发, 林楚雄, 黄晓锋, 何凌燕. 深圳市冬季大气中硝酸分配特征观测研究[J]. 中国环境科学, 2023, 43(8): 3877-3885. LUO Yao, LIN Xiao-yu, NIU Ying-bo, YUN Long, GU Tian-fa, LIN Chu-xiong, HUANG Xiao-feng, HE Ling-yan. Observation of partitioning characteristics of gaseous nitric acid in winter of Shenzhen. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(8): 3877-3885.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2023/V43/I8/3877

[1]	Cohen A J, Brauer M, Burnett R, et al. Estimates and 25-year trends of the global burden of disease attributable to ambient air pollution:an analysis of data from the Global Burden of Diseases Study 2015[J]. Lancet, 2017,389(10082):1907-1918.
[2]	Wang Q, Wang J, Zhou J, et al. Estimation of PM2.5-associated disease burden in China in 2020 and 2030 using population and air quality scenarios:a modelling study[J]. Lancet Planet Health, 2019,3:71-80.
[3]	Hu S, Zhao G, Tan T, et al. Current challenges of improving visibility due to increasing nitrate fraction in PM2.5 during the haze days in Beijing, China[J]. Environmental Pollution, 2021,290:118032.
[4]	TenBrink H M, Veefkind J P, Waijers-Ijpelaan A, et al. Aerosol light-scattering in The Netherlands[J]. Atmospheric Environment, 1996,30(24):4251-4261.
[5]	Nenes A, Pandis S N, Kanakidou M, et al. Aerosol acidity and liquid water content regulate the dry deposition of inorganic reactive nitrogen[J]. Atmospheric Chemistry and Physics, 2021,21(8):6023-6033.
[6]	Ye C, Zhang N, Gao H, et al. Photolysis of Particulate Nitrate as a Source of HONO and NOx[J]. Environmental Science & Technology, 2017,51(12):6849-6856.
[7]	Peng X, Wang T, Wang W, et al. Photodissociation of particulate nitrate as a source of daytime tropospheric Cl2[J]. Nature Communications, 2022,13.
[8]	Li R, Cui L, Zhao Y, et al. Long-term trends of ambient nitrate (NO3-) concentrations across China based on ensemble machine-learning models[J]. Earth System Science Data, 2021,13(5):2147-2163.
[9]	Wen L, Xue L, Wang X, et al. Summertime fine particulate nitrate pollution in the North China Plain:increasing trends, formation mechanisms and implications for control policy[J]. Atmospheric Chemistry and Physics, 2018,18(15):11261-11275.
[10]	Kong L, Feng M, Liu Y, et al. Elucidating the pollution characteristics of nitrate, sulfate and ammonium in PM2.5 in Chengdu, southwest China, based on 3-year measurements[J]. Atmospheric Chemistry and Physics, 2020,20(19):11181-11199.
[11]	Yun H, Wang W, Wang T, et al. Nitrate formation from heterogeneous uptake of dinitrogen pentoxide during a severe winter haze in southern China[J]. Atmospheric Chemistry and Physics, 2018,18(23):17515-17527.
[12]	Chen X, Wang H, Lu K, et al. Field Determination of Nitrate Formation Pathway in Winter Beijing[J]. Environmental Science & Technology, 2020,54(15):9243-9253.
[13]	Fu X, Wang T, Gao J, et al. Persistent Heavy Winter Nitrate Pollution Driven by Increased Photochemical Oxidants in Northern China[J]. Environmental Science & Technology, 2020,54(7):3881-3889.
[14]	Zhai S, Jacob D J, Wang X, et al. Control of particulate nitrate air pollution in China[J]. Nature Geoscience, 2021,14(6):389-395.
[15]	Guo H, Liu J, Froyd K, et al. Fine particle pH and gas-particle phase partitioning of inorganic species in Pasadena, California, during the 2010 CalNex campaign[J]. Atmospheric Chemistry and Physics, 2017,17(9):5703-5719.
[16]	Prabhakar G, Parworth C, Zhang X, et al. Observational assessment of the role of nocturnal residual-layer chemistry in determining daytime surface particulate nitrate concentrations[J]. Atmospheric Chemistry and Physics, 2017,17(23):14747-14770.
[17]	Liu L, Zhang X, Zhang Y, et al. Dry Particulate Nitrate Deposition in China[J]. Environmental Science & Technology, 2017,51(10):5572-5581.
[18]	Shi X, Nenes A, Xiao Z, et al. High-resolution data sets unravel the effects of sources and meteorological conditions on nitrate and its gas-particle partitioning[J]. Environmental Science & Technology, 2019,53(6):3048-3057.
[19]	Shah V, Jaegle L, Thornton J A, et al. Chemical feedbacks weaken the wintertime response of particulate sulfate and nitrate to emissions reductions over the eastern United States[J]. Proceedings of the National Academy of Sciences, 2018,115(32):8110-8115.
[20]	Battaglia Jr M A, Balasus N, Ball K, et al. Urban aerosol chemistry at a land-water transition site during summer-Part 2:Aerosol pH and liquid water content[J]. Atmospheric Chemistry and Physics, 2021, 21(24):18271-18281.
[21]	Zang H, Zhao Y, Huo J, et al. High atmospheric oxidation capacity drives wintertime nitrate pollution in the eastern Yangtze River Delta of China[J]. Atmospheric Chemistry and Physics, 2022,22(7):4355-4374.
[22]	Huang X, Zou B, He L, et al. Exploration of PM2.5 sources on the regional scale in the Pearl River Delta based on ME-2 modeling[J]. Atmospheric Chemistry and Physics, 2018,18(16):11563-11580.
[23]	陈雪,黄晓锋,朱波,等.深圳市秋季VOCs空间分布特征与关键减排物种[J].中国环境科学, 2021,41(9):4069-4076. Chen X, Huang X F, Zhu B, et al. Spatial distribution characteristics of VOCs and key emission reduction species in autumn Shenzhen[J]. China Environmental Science, 2021,41(9):4069-4076.
[24]	江家豪,彭杏,朱波,等.深圳大气PM2.5化学组成的长期变化特征[J].中国环境科学, 2021,41(2):574-579. Jiang J H, Peng X, Zhu B, et al. Long-term variational characteristics of the chemical composition of PM2.5 in Shenzhen[J]. China Environmental Science, 2021,41(2):574-579.
[25]	张明棣,何冬一,古添发,等.深圳市道路交通源温室气体排放特征分析[J].中国环境科学, 2022,42(4):1518-1525. Zhang M D, He D Y, Gu T F, et al. The characterization of greenhouse gas emission from road traffic sources in Shenzhen[J]. China Environmental Science, 2022,42(4):1518-1525.
[26]	古添发,闫润华,姚沛廷,等.深圳市大气中PM2.5载带金属污染特征及健康风险[J].中国环境科学, 2022,43(1):88-95. Gu T F, Yan R H, Yao P T, et al. Characteristics and health risks of PM2.5-bound metals in the air of road environment in Shenzhen[J]. China Environmental Science, 2022,43(1):88-95.
[27]	Rumsey I C, Cowen K A, Walker J T, et al. An assessment of the performance of the Monitor for AeRosols and GAses in ambient air (MARGA):a semi-continuous method for soluble compounds[J]. Atmospheric Chemistry and Physics, 2014,14(11):5639-5658.
[28]	Makkonen U, Virkkula A, Mäntykenttä J, et al. Semi-continuous gas and inorganic aerosol measurements at a Finnish urban site:comparisons with filters, nitrogen in aerosol and gas phases, and aerosol acidity[J]. Atmospheric Chemistry and Physics, 2012,12(12):5617-5631.
[29]	Villena G, Bejan I, Kurtenbach R, et al. Interferences of commercial NO2instruments in the urban atmosphere and in a smog chamber[J]. Atmospheric Measurement Techniques, 2012,5(1):149-159.
[30]	Hennigan C J, Izumi J, Sullivan A P, et al. A critical evaluation of proxy methods used to estimate the acidity of atmospheric particles[J]. Atmospheric Chemistry and Physics, 2015,15(5):2775-2790.
[31]	Rindelaub J D, Craig R L, Nandy L, et al. Direct Measurement of pH in Individual Particles via Raman Microspectroscopy and Variation in Acidity with Relative Humidity[J]. Journal of Physical Chemistry A, 2016,120(6):911-917.
[32]	Song Q, Osada K. Direct measurement of aerosol acidity using pH testing paper and hygroscopic equilibrium under high relative humidity[J]. Atmospheric Environment, 2021,261.
[33]	Fountoukis C, Nenes A. ISORROPIA II:a computationally efficient thermodynamic equilibrium model for K+-Ca2+-Mg2+-NH4+-Na+-SO42−-NO3−-Cl−-H2O aerosols[J]. Atmospheric Chemistry and Physics, 2007,7(1):4639-4659.
[34]	Guo H, Xu L, Bougiatioti A, et al. Fine-particle water and pH in the southeastern United States[J]. Atmospheric Chemistry and Physics, 2015,15(9):5211-5228.
[35]	Liu Y, Wu Z, Huang X, et al. Aerosol phase state and its link to chemical composition and liquid water content in a subtropical coastal megacity[J]. Environmental Science & Technology, 2019,53(9):5027-5033.
[36]	Jia S, Wang X, Zhang Q, et al. Technical note:Comparison and interconversion of pH based on different standard states for aerosol acidity characterization[J]. Atmospheric Chemistry and Physics, 2018, 18(15):11125-11133.
[37]	Pye H O T, Zuend A, Fry J L, et al. Coupling of organic and inorganic aerosol systems and the effect on gas-particle partitioning in the southeastern US[J]. Atmospheric Chemistry and Physics, 2018,18(1):357-370.
[38]	Battaglia Jr M A, Weber R J, Nenes A, et al. Effects of water-soluble organic carbon on aerosol pH[J]. Atmospheric Chemistry and Physics, 2019,19(23):14607-14620.
[39]	许重光,尹强,邹冰,等.深圳市城市总体规划(2010~2020)建设用地布局规划图[EB/OL]. https://www.szcaupd.com/project-ztghi_11235.htm, 2010. Xu C Z, Yin Q, Zou B, et al. Shenzhen City master plan (2010~2020) construction land layout planning map[EB/OL]. https://www.szcaupd.com/project-ztghi_11235.htm, 2010.
[40]	孙天乐,何冬一,林晓玉,等.深圳市不同区域大气CO2浓度变化特征与来源分析[J].中国环境科学, 2022,42:5497-5505. Sun T L, He D Y, Lin X Y, et al. The characterization and source analysis of atmospheric CO2 in different areas of Shenzhen[J]. China Environmental Science, 2022,42:5497-5505.
[41]	江家豪.深圳大气PM2.5来源的长期演变特征[D].北京:北京大学, 2021. Jiang J H. Long-term evolution characteristics of atmospheric PM2.5 sources in Shenzhen[D]. BeiJing:Peking University, 2021.
[42]	林楚雄,姚沛廷,彭杏,等.深圳市城区冬季大气PM2.5在线来源解析[J].中国环境科学, 2022,43:506-513. Lin C X, Yao P T, Peng X, et al. Online source apportionment of PM2.5during winter at urban site in Shenzhen[J]. China Environmental Science, 2022,43:506-513.
[43]	Ding J, Zhao P, Su J, et al. Aerosol pH and its driving factors in Beijing[J]. Atmospheric Chemistry and Physics, 2019,19(12):7939-7954.
[44]	Fu Z, Cheng L, Ye X, et al. Characteristics of aerosol chemistry and acidity in Shanghai after PM2.5 satisfied national guideline:Insight into future emission control[J]. Sci Total Environ, 2022,827:154319.
[45]	Zhang B, Shen H, Liu P, et al. Significant contrasts in aerosol acidity between China and the United States[J]. Atmospheric Chemistry and Physics, 2021,21(10):8341-8356.
[46]	Guo H, Nenes A, Weber R J. The underappreciated role of nonvolatile cations in aerosol ammonium-sulfate molar ratios[J]. Atmospheric Chemistry and Physics, 2018,18(23):17307-17323.
[47]	Guo H, Sullivan A P, Campuzano-Jost P, et al. Fine particle pH and the partitioning of nitric acid during winter in the northeastern United States[J]. Journal of Geophysical Research:Atmospheres, 2016,121(17):10355-10376.
[48]	Gao X, Yang L, Cheng S, et al. Semi-continuous measurement of water-soluble ions in PM2.5 in Jinan, China:Temporal variations and source apportionments[J]. Atmospheric Environment, 2011,45(33):6048-6056.
[49]	Tan Z, Wang H, Lu K, et al. An observational based modeling of the surface layer particulate nitrate in the North China Plain during summertime[J]. Journal of Geophysical Research:Atmospheres, 2021,126(18):e2021JD035623.
[50]	Niu Y, Huang X, Wang H, et al. Effects of nighttime heterogeneous reactions on the formation of secondary aerosols and ozone in the Pearl River Delta[J]. Chinese Science Bulletin, 2021,67(18):2060-2068.
[51]	Huang D D, Zhu S, An J, et al. Comparative assessment of cooking emission contributions to urban organic aerosol using online molecular tracers and aerosol mass spectrometry measurements[J]. Environmental Science & Technology, 2021,55(21):14526-14535.
[52]	Bougiatioti A, Nikolaou P, Stavroulas I, et al. Particle water and pH in the eastern Mediterranean:source variability and implications for nutrient availability[J]. Atmospheric Chemistry and Physics, 2016, 16(7):4579-4591.
[53]	Zheng G, Wang S, Andreae M O, et al. Multiphase buffer theory explains contrasts in atmospheric aerosol acidity[J]. Science, 2020, 369(6509):1374-1377.
[54]	Clegg S L, Brimblecombe P. Equilibrium partial pressures and mean activity and osmotic coefficients of 0-100-percent nitric-acid as a function of temperature[J]. J Phys Chem, 1990,94(13):5369-5380.
[55]	陈瑶,云龙,罗遥,等.深圳冬季大气气态硝酸和硝酸盐气粒分配特征[J].中国环境科学, 2021,41(9):4036-4042. Chen Y, Yun L, Luo Y, et al. Characteristics of gas-particle partitioning of gaseous nitric acid and particle nitrate in Shenzhen in winter[J]. China Environmental Science, 2021,41(9):4036-4042.
[56]	云龙,牛英博,罗遥,等.深圳市冬季夜间大气中N2O5污染特征[J].中国环境科学, 2022,42:5506-5513. Yun L, Niu Y B, Luo Y, et al. The characterization of nocturnal dinitrogen pentoxide pollution in winter of Shenzhen[J]. China Environmental Science, 2022,42:5506-5513.
[57]	Wang Y, Chen Y, Wu Z, et al. Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility[J]. Atmospheric Chemistry and Physics, 2020,20(4):2161-2175.
[58]	Tan H, Cai M, Fan Q, et al. An analysis of aerosol liquid water content and related impact factors in Pearl River Delta[J]. Science of The Total Environment, 2017,579:1822-1830.
[59]	Abbatt J P, Lee A K, Thornton J A. Quantifying trace gas uptake to tropospheric aerosol:recent advances and remaining challenges[J]. Chemical Society Reviews, 2012,41(19):6555-6581.
[60]	Bertram T H, Thornton J A, Riedel T P, et al. Direct observations of N2O5reactivity on ambient aerosol particles[J]. Geophysical Research Letters, 2009,36(19):L19803.
[61]	Cheng Y, Zheng G, Wei C, et al. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China[J]. Science Advances, 2016,2(12):e1601530.
[62]	Wang G, Zhang R, Gomez M E, et al. Persistent sulfate formation from London Fog to Chinese haze[J]. Proceedings of the National Academy of Sciences, 2016,113(48):13630-13635.
[63]	Hennigan C J, Bergin M H, Dibb J E, et al. Enhanced secondary organic aerosol formation due to water uptake by fine particles[J]. Geophysical Research Letters, 2008,35(18):L18801.
[64]	Faust J A, Wong J P, Lee A K, et al. Role of aerosol liquid water in secondary organic aerosol formation from volatile organic compounds[J]. Environmental Science & Technology, 2017,51(3):1405-1413.
[65]	Wu Z, Wang Y, Tan T, et al. Aerosol liquid water driven by anthropogenic inorganic salts:Implying its key role in haze formation over the North China Plain[J]. Environmental Science & Technology Letters, 2018,5(3):160-166.
[66]	Chen C, Zhang H, Yan W, et al. Aerosol water content enhancement leads to changes in the major formation mechanisms of nitrate and secondary organic aerosols in winter over the North China Plain[J]. Environmental Pollution, 2021,287:117625.
[67]	Tao Y, Murphy J G. The sensitivity of PM2.5acidity to meteorological parameters and chemical composition changes:10-year records from six Canadian monitoring sites[J]. Atmospheric Chemistry and Physics, 2019,19(14):9309-9320.
[68]	Tao Y, Murphy J G. Simple framework to quantify the contributions from different factors influencing aerosol pH based on NHx phase-partitioning equilibrium[J]. Environmental Science & Technology, 2021,55(15):10310-10319.
[69]	Jia S, Chen W, Zhang Q, et al. A quantitative analysis of the driving factors affecting seasonal variation of aerosol pH in Guangzhou, China[J]. Science of the Total Environment, 2020,725.