青岛总悬浮颗粒物中水溶性离子的时间变化、来源解析和环境效应

李逗; 王艳; 刘汝海; 孙浩麟; 尹萍萍; 周续缘; 莫冰; 李冬婷

doi:10.13205/j.hjgc.202308014

青岛总悬浮颗粒物中水溶性离子的时间变化、来源解析和环境效应

doi: 10.13205/j.hjgc.202308014

李逗^1,2,
王艳^1,2,
刘汝海^1,2, ,,
孙浩麟^1,2,
尹萍萍^1,2,
周续缘^1,2,
莫冰^1,2,
李冬婷^1,2

1. 中国海洋大学环境科学与工程学院, 山东青岛 266100;
2. 中国海洋大学海洋环境与生态教育部重点实验室, 山东青岛 266100

基金项目:

山东省自然科学基金项目(ZR2020MD118,ZR2018MD004)

国家自然科学基金项目(41506128)

详细信息

作者简介:
李逗(1997-),女,硕士,主要研究方向为大气环境化学。1742888219@qq.com

通讯作者:
刘汝海(1975-),男,副教授,主要从事污染元素生物地球化学循环研究。ruhai@ouc.edu.cn

计量
- 文章访问数: 101
- HTML全文浏览量: 15
- PDF下载量: 3
- 被引次数: 0
出版历程
- 收稿日期: 2022-11-24
- 网络出版日期: 2023-11-15

TEMPORAL VARIATION, SOURCE ANALYSIS AND ENVIRONMENTAL EFFECTS OF WATER-SOLUBLE IONS IN TSP IN QINGDAO

LI Dou^1,2,
WANG Yan^1,2,
LIU Ruhai^{1,2
, ,},
SUN Haolin^1,2,
YIN Pingping^1,2,
ZHOU Xuyuan^1,2,
MO Bing^1,2,
LI Dongting^1,2

1. College of Environmental Science and Engineering, Ocean University of China, Qingdao 266100, China;
2. Key Laboratory of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao 266100, China

摘要

摘要: 为揭示青岛大气污染变化特征及其向近海营养物质的输送,对其大气颗粒物中水溶性组分进行长期研究。于2019-11—2021-04期间采集总悬浮颗粒物(TSP)样品,测定了 9种水溶性无机离子(WSIIs)含量,研究其时间变化、来源和环境效应。结果表明:青岛市TSP中ρ(WSIIs)为(32.0±6.51) μg/m³,主要离子为NO^-₃、SO^2-₄和NH⁺₄,2013年后受能源结构调整和污染防控政策影响,SO^2-₄浓度明显下降,NO^-₃浓度增加。NO^-₃和NH⁺₄浓度呈冬季＞春季＞秋季＞夏季,SO^2-₄浓度呈冬季＞夏季＞春季＞秋季,夏季太阳辐射强、气温高,NO^-₃和NH⁺₄易于分解和挥发使其浓度最低;冬季受来自蒙古和华北的内陆气团、燃煤供暖和不利的大气扩散条件影响,WSIIs浓度最高;夏季强太阳辐射利于SO^2-₄的生成,同时夏季风使海源性硫酸盐输入增加,导致SO^2-₄浓度偏高。年均ρ(NO^-₃)/ρ(SO^2-₄)比值>1,以移动源污染为主;各季节SOR、NOR均>0.1,氮、硫的二次生成率较高。NH⁺₄-N、NO^-₃-N营养盐的沉降通量分别为48.8,87.0 mmol/(m²·a),氮沉降通量的相对升高将加剧近海浮游植物生长的磷限制。
- 总悬浮颗粒物 /
- 水溶性离子 /
- 季节变化 /
- 来源分析 /
- 氮沉降
Abstract: A long-term study of water-soluble fractions in atmospheric particulate matter in Qingdao was conducted to reveal the characteristics of atmospheric pollution changes and their nutrient transportation to offshore. Total suspended particulate matter (TSP) samples were collected from 2019-11 to 2021-04, and the contents of nine water soluble inorganic ions (WSIIs) were measured to evaluated their temporal changes, sources, and environmental effects. The results showed that the concentration of WSIIs in Qingdao TSP was (32.0±6.51) μg/m³, and the main ions were NO₃^-, SO₄^2- and NH₄⁺. After 2013, influenced by energy structure adjustment and pollution prevention and control policies, the concentration of SO₄^2- decreased significantly and the concentration of NO₃^- increased. The concentration of NO₃^- and NH₄⁺ was in the order of winter>spring>autumn>summer, and the concentration of SO₄^2- was in the order of winter>summer>spring>autumn. With strong solar radiation and high temperature in summer, NO₃^- and NH₄⁺ were easily decomposed and volatilized, resulting in the lowest concentrations in summer; WSIIs concentrations were highest in winter due to inland air masses transportation from Mongolia and North China, coal heating and unfavorable atmospheric dispersion conditions; strong solar radiation in summer facilitated SO₄^2- production, while summer winds increased sea-sourced sulfate input, resulting in high SO₄^2- concentrations in summer. The annual average ρ(NO₃^-)/ρ(SO₄^2-) ratio was greater than 1, and mobile source pollution was dominant; SOR and NOR were greater than 0.1 in all seasons, and secondary production rates of nitrogen and sulfur were high. Sink fluxes of NH₄⁺-N and NO₃^--N nutrients were 48.8, 87.0 mmol/(m²·a), respectively, and the relative increase in nitrogen sink fluxes would exacerbate the phosphorus limitation of offshore phytoplankton growth.
- TSP /
- water-soluble ions /
- seasonal changes /
- source analysis /
- nitrogen deposition

HTML全文

参考文献(40)

[1]	LEE S B,BAE G N,MOON K C,et al.Characteristics of TSP and PM_2.5 measured at Tokchok Island in the Yellow Sea[J].Atmospheric Environment,2002,36:5427-5435.
[2]	HOFFMANN D,TILGNER A,IINUMA Y,et al.Atmospheric stability of levoglucosan:a detailed laboratory and modeling study[J].Environmental Science & Technology,2010,44(2):694-699.
[3]	ZHAN Y A,TSONA N T,LI J L,et al.Water-soluble matter in PM_2.5 in a coastal city over China:chemical components,optical properties,and source analysis[J].Journal of Environmental Sciences,2022,114:21-36.
[4]	刘臻,祁建华,王琳,等.青岛大气气溶胶水溶性无机离子研究:季节分布特征[J].环境科学,2012,33(7):2180-2190.
[5]	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.
[6]	张宁宁,何元庆,王春凤,等.丽江市冬季大气总悬浮颗粒物(TSP)中水溶性离子化学特征[J].环境科学,2011,32(3):619-625.
[7]	陶俊,陈刚才,钟昌琴.重庆市大气TSP中水溶性无机离子的化学特征[J].中国环境监测,2006,22(6):71-74.
[8]	ZHOU Q Y,ZHANG L L,YANG L,et al.Long-term variability of inorganic ions in TSP at a remote background site in Japan (Wajima) from 2005 to 2015[J].Chemosphere,2021,264:128427.
[9]	ZHANG T,CAO J J,TIE X X,et al.Water-soluble ions in atmospheric aerosols measured in Xi’an,China:seasonal variations and sources[J].Atmospheric Research,2011,102(1/2):110-119.
[10]	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.
[11]	方言,曹芳,范美益,等.中国东海近海岛屿冬季与夏季气溶胶中水溶性离子化学组分特征及来源解析[J].环境科学,2020,41(3):1025-1035.
[12]	SCIARE J,OIKONOMOU K,CACHIER H,et al.Aerosol mass closure and reconstruction of the light scattering coefficient over the Eastern Mediterranean Sea during the MINOS campaign[J].Atmospheric Chemistry and Physics,2005,5:2253-2265.
[13]	SHON Z,GHOSH S,KIM K,et al.Analysis of water-soluble ions and their precursor gases over diurnal cycle[J].Atmospheric Research,2013,132/133:309-321.
[14]	QIAO T,ZHAO M F,XIU G L,et al.Seasonal variations of water soluble composition (WSOC,Hulis and WSIIs) in PM₁ and its implications on haze pollution in urban Shanghai,China[J].Atmospheric Environment,2015,123:306-314.
[15]	陈晓静.青岛沿海大气气溶胶中水溶性离子和金属元素的分布特征及其来源解析[D].青岛:中国海洋大学,2014.
[16]	姚青,孙玫玲,张长春,等.潮州沿海大气气溶胶无机离子浓度分布与气象要素的相关分析[J].气象与环境学报,2007,23(4):39-42.
[17]	SI Y D,YU C,ZHANG L,et al.Assessment of satellite-estimated near-surface sulfate and nitrate concentrations and their precursor emissions over China from 2006 to 2014[J].Science of the Total Environment,2019,669:362-376.
[18]	韩琨,刘汝海,徐红霞,等.青岛市降尘中水溶性离子的特征以及来源分析[J].环境工程,2022,40(3):111-117.
[19]	王珉,胡敏.青岛沿海地区大气气溶胶浓度与主要无机化学组成[J].环境科学,2001,22(1):6-9.
[20]	闫文蕊.海盐气溶胶对天津大气颗粒物的贡献研究[D].天津:天津师范大学,2022.
[21]	CHONG X X,WANG Y,ZHANG Y Q,et al.Variation characteristics and source differences of gaseous elemental mercury over four seasons in Qingdao:influence of weather processes[J].Atmospheric Environment,2020,222:117118.
[22]	邹玉玲,刘朝晖,马亚维,等.青岛低空逆温层特征分析[J].山东气象,2007,27(1):28-29.
[23]	DONG Z S,SU F C,ZHANG Z Y,et al.Observation of chemical components of PM_2.5 and secondary inorganic aerosol formation during haze and sandy haze days in Zhengzhou,China[J].Journal of Environmental Sciences,2020,88:316-325.
[24]	HE Q S,YAN Y L,GUO L L,et al.Characterization and source analysis of water-soluble inorganic ionic species in PM_2.5 in Taiyuan city,China[J].Atmospheric Research,2017,184:48-55.
[25]	YANG G P,JING W W,KANG Z Q,et al.Spatial variations of dimethylsulfide and dimethylsulfoniopropionate in the surface microlayer and in the subsurface waters of the South China Sea during springtime[J].Marine Environmental Research,2008,65(1):85-97.
[26]	ALVI M U,KISTLER M,MAHMUD T,et al.The composition and sources of water soluble ions in PM₁₀ at an urban site in the Indo-Gangetic Plain[J].Journal of Atmospheric and Solar-Terrestrial Physics,2019,196:105142.
[27]	HSU S C,LIU S C,KAO S J,et al.Water-soluble species in the marine aerosol from the northern South China Sea:high chloride depletion related to air pollution[J].Journal of Geophysical Research,2007,112(D19):304-315.
[28]	ZHANG X Y,ZHAO X,JI G X,et al.Seasonal variations and source apportionment of water-soluble inorganic ions in PM_2.5 in Nanjing,a megacity in southeastern China[J].Journal of Atmospheric Chemistry,2019,76(1):73-88.
[29]	WANG X F,WANG W X,YANG L X,et al.The secondary formation of inorganic aerosols in the droplet mode through heterogeneous aqueous reactions under haze conditions[J].Atmospheric Environment,2012,63:68-76.
[30]	王碧菡,廖婷婷,车红蕾,等.成都西南郊区大气PM₁中水溶性离子季节变化特征[J].环境工程,2022,40(9):26-32.
[31]	任娇,尹诗杰,郭淑芬.太原市大气PM_2.5中水溶性离子的季节污染特征及来源分析[J].环境科学学报,2020,40(9):3120-3130.
[32]	XIU G L,ZHANG D N,CHEN J Z,et al.Characterization of major water-soluble inorganic ions in size-fractionated particulate matters in Shanghai campus ambient air[J].Atmospheric Environment,2004,38(2):227-236.
[33]	CAO J J,SHEN Z X,CHOW J C,et al.Winter and summer PM_2.5 chemical compositions in fourteen Chinese cities[J].Journal of the Air & Waste Management Association,2012,62(10):1214-1226.
[34]	丁淑琴,吴家平,万学平,等.常熟市秋冬季典型大气重污染过程中PM_2.5及其主要化学组分分析[J].环境工程,2020,38(3):142-149.
[35]	WANG Y,ZHUANG G S,ZHANG X Y,et al.The ion chemistry,seasonal cycle,and sources of PM_2.5 and TSP aerosol in Shanghai[J].Atmospheric Environment,2006,40(16):2935-2952.
[36]	CARBO P,KROM M D,HOMOKY W B,et al.Impact of atmospheric deposition on N and P geochemistry in the southeastern Levantine basin[J].Deep Sea Research Part Ⅱ:Topical Studies in Oceanography,2005,52(22/23):3041-3053.
[37]	姜晓璐.东、黄海的大气干、湿沉降及其对海洋初级生产力的影响[D].青岛:中国海洋大学,2009.
[38]	KIM T W,LEE K,NAJJAR R G,et al.Increasing N abundance in the Northwestern Pacific Ocean due to atmospheric nitrogen deposition[J].Science,2011,334(6055):505-509.
[39]	高会旺,姚小红,郭志刚,等.大气沉降对海洋初级生产过程与氮循环的影响研究进展[J].地球科学进展,2014,29(12):1325-1332.
[40]	郭伟,史洁,朱君莹,等.大气氮沉降对南黄海初级生产过程影响的数值研究[J].中国海洋大学学报(自然科学版),2020,50(1):115-125.