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作者简介:

郭庆皓,男,硕士生,主要研究方向为大气物理学与大气环境.G_qinghao@163.com;

陈魁(通信作者),男,博士,副教授,研究方向为大气成分及气候效应.ch_k@163.com

中图分类号:X511

文献标识码:A

DOI:10.13878/j.cnki.jnuist.2022.03.005

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目录contents

    摘要

    基于2015年1月1日—2021年2月10日南京市大气污染物监测数据,分析了南京市主要大气污染物时空分布特征与潜在源区贡献.结果表明:1)近6年南京市6种大气污染物(CO、NO2、SO2、O3、PM10和PM2.5)年均质量浓度分别为800、43.1、13.0、106.0、77.1和43.0 μg·m-3;南京臭氧质量浓度均值高于中国典型城市(北京、上海、广州、成都、兰州和武汉),而PM2.5平均质量浓度最低.2)2015—2020年南京NO2、PM10和PM2.5超标天数呈减少趋势,平均降低率分别为29.1%、38.1%和28.1%,而臭氧超标天数呈增加趋势;臭氧季节变化表现出夏高冬低,其他5种污染物均呈现冬季高特征.3)冬季(特别是1月)南京PM2.5质量浓度均值最高,对该时间段南京细颗粒物进行潜在源分析,发现南京地区细颗粒物主要受周边工业污染物输送影响,安徽、江苏北部和山东为主要潜在源区.4)对比研究了2019、2020和2021年1—2月大气污染物情况,发现2020年南京大气污染物质量浓度最低,说明因新冠疫情采取的封控措施减少了人类活动,进而显著影响了环境空气质量.

    Abstract

    Based on monitoring data of atmospheric pollutants in Nanjing from Jan.1,2015 to Feb.10,2021,the spatial-temporal distribution characteristics of Nanjing's ambient air quality and the contribution of potential source areas were analyzed.The average concentrations of six air pollutants (CO,NO2,SO2,O3,PM10,and PM2.5) were 800 μg·m-3,43.1 μg·m-3,13.0 μg·m-3,106.0 μg·m-3,77.1 μg·m-3,and 43.0 μg·m-3,respectively.The average concentration of ozone in Nanjing was higher than that in China's other typical cities (Beijing,Shanghai,Guangzhou,Chengdu,Lanzhou,and Wuhan).The number of pollution days for NO2,PM10,and PM2.5 were reduced by 29.1%,38.1%,and 28.1% during 2015 to 2020.However,the frequency of ozone pollution days was increasing (the highest value in summer and the lowest value in winter).The potential source analysis of fine particulate matter in January of 2015-2020 was carried out.It was found that the potential source for Nanjing's PM2.5 was surrounding industrial areas (Anhui province,north of Jiangsu province,and Shandong province).The concentration of air pollutants in Nanjing in 2020 was lower than that in 2019 and 2021.It indicated that the reduction of human activity caused by COVID-19 pandemic has resulted in less air pollutant emissions and improved air quality in Nanjing.

  • 0 引言

  • 近年来,伴随城市快速发展和工业化进程加快,机动车和工业排放大幅增加,我国大气环境逐渐形成了一次和二次污染物并存的复合型污染[1-2].许多城市地区由于颗粒物质量浓度高导致能见度下降和灰霾加重,且人为排放过多的氮氧化物(NOx)、挥发性有机物(VOCs)等前体物通过光化学反应引起臭氧污染加剧,严重损害人体健康,对生态环境与天气气候[3-6]产生重要影响.因此,我国大气环境面临挑战,研究环境空气质量特征变化是我国大气污染治理工作的重要基础.

  • 城市环境空气质量极易受到人为排放污染和气象状态影响,人为排放影响着区域大气污染程度,气象条件密切关联着大气污染物的扩散和清除能力[7-8].从2013年1月开始,全国主要城市空气质量监测站发布大气污染物小时平均质量浓度数据,出版了大量空气质量相关研究文献,主要研究区域集中在京津冀、长三角、珠三角和成渝地区[9].例如,徐冉等[10]分析北京秋冬两季重污染时期大气污染物浓度水平和气团传输的影响,指出冬季发生重污染程度高于秋季.舒卓智等[11]研究云贵高原城市空气污染特征,发现该地区近地面O3质量浓度呈逐年上升趋势.陈优良等[12]发现长三角地区空气质量空间分布呈现经济发达的城市臭氧质量浓度较高的特征.徐鹏等[13]阐述了重庆北碚区的大气污染状况,发现不同季节污染物和气象要素相关性表现不同.王爱平等[14]讨论了2020年疫情期间南京空气质量改善情况,指出人为减排对大气污染有着明显影响.由于环境空气质量的长期演变特征能够反映出该地区大气污染的特性,因此,分析大气污染物长期特征以及潜在污染源有助于大气环境治理.

  • 南京市是长三角地区典型城市(2019年末南京的常住人口达到850万人),城镇化率为83.2%,聚集了南钢和扬子石化等重工业企业,工业能源消费仍然以煤炭为主[15-16].此外,南京属北亚热带湿润气候,夏季闷热多雨,而冬季干燥,容易出现逆温现象[17],不利于大气污染物沉降和扩散.近年来南京市对大气污染物加强管控[18],采取限制机动车排放和改进工业生产工艺等措施,环境空气质量得到改善,但以臭氧为主要污染物的二次混合型污染问题日益突出[19-21].

  • 本文利用2015年1月1日—2021年2月10日南京市空气质量国控站的空气质量数据,分析南京市大气污染物的质量浓度水平和污染特征,以及气象条件对大气污染物的作用,研究南京市PM2.5的潜在污染源区,并探讨了2019、2020和2021年1—2月(2020年新冠疫情封控期)大气污染物状况,获得人为活动减少对大气污染物改变的确切原因,以期为改善南京城市空气质量和制订更为合理大气污染控制措施提供科学依据.

  • 1 资料与方法

  • 1.1 数据来源

  • 本文选取南京市环境空气质量国控站2015年1月1日—2021年2月10日的监测资料,包括大气环境主要污染物:CO、NO2、SO2、O3_8h(8h平均臭氧质量浓度)、PM10和PM2.5每日逐小时质量浓度,数据来源于中国国家环境监测中心网站(http://www.cnemc.cn/).南京市环境空气质量国控站和气象观测站位置和分布情况如图1所示.同期南京市气象观测站地面观测数据包括温度(℃)、相对湿度(%)、风速(m·s-1)、降水量(mm),来源于美国国家环境信息中心(https://www.ngdc.noaa.gov/)小时分辨率资料.

  • 1.2 研究方法

  • 1.2.1 潜在源分析

  • 本研究潜在源分析主要采用潜在源贡献分析法(Potential Source Contribution Function,PSCF)和质量浓度权重分析法(Concentration Weighted Trajectory,CWT).PSCF是基于后向轨迹确定污染源区的一种方法,PCSFij值定义为在研究区域内,经过网格(i,j)超过质量浓度阈值的轨迹数(mij )和经过网格(i,j)的轨迹总数(nij )之比,其公式为

  • PSCFij=mijnij.
    (1)
  • 鉴于PSCF是一个概率函数(fPSCF),若nij值较小会导致不确定性增大,为降低这种不确定性,引入权重函数Wij,其公式为

  • WPSCF=Wij×fPSCF
    (2)
  • PSCF方法只能反映污染轨迹经过各网格的概率,CWT则可反映轨迹的污染程度.通过网格的平均权重质量浓度来确定其对该网格的污染贡献,其公式为

  • Cij=i=1M Cl×Tijli=1M Tijl
    (3)
  • 式(3)中,Cij是网格(i,j)上的平均权重质量浓度(μg·m-3),M是轨迹总数(条),Cl是轨迹l经过网格(i,j)时污染物质量浓度(μg·m-3),Tijl是轨迹l在网格(i,j)的停留时间.CWT方法也需要使用权重函数Wij来消除不确定性,修正后的质量浓度权重值为

  • WCWT=Wij×Cij
    (4)
  • 1.2.2 疫情时间划分

  • 2020年春节前后爆发新型冠状病毒(COVID-19)疫情,为了解南京实施疫情管控措施对空气污染的影响,根据国务院发布的《国家突发公共事件应急预案》和实际疫情发展情况,设1月10—24日共15d为疫情封控前时期,1月25—2月10日共17d为疫情封控期.封控期内停止集市、集会等大型活动,公共场所市民人数显著减少,工业企业、建筑工地、餐饮企业等大规模停工停业.因此本文研究以2020年1月25日—2月10日作为疫情封控期,分析人为活动改变对大气污染状况的影响.

  • 图1 南京市空气质量监测站及气象观测点分布

  • Fig.1 Distribution of air quality monitoring stations and a meteorological observation site in Nanjing

  • 2 结果与讨论

  • 2.1 大气污染总体情况

  • 图2展示了2015年1月1日—2021年2月10日南京市主要大气污染物质量浓度情况.CO、NO2、SO2、O3_8h、PM10和PM2.5平均质量浓度分别为800、43.1、13.0、106.0、77.1和43.0 μg·m-3,最大值分别为2 200、126.2、71.6、280.0、381.1和256.1 μg·m-3,其中PM2.5质量浓度最大值远高于国家环境空气质量标准质量浓度限值(一级标准35 μg·m-3和二级标准75 μg·m-3),表明研究期内南京有极端颗粒物污染事件发生.

  • 图2 南京市主要污染物质量浓度

  • Fig.2 Concentration of major air pollutants in Nanjing

  • 对比我国其他典型城市大气污染物质量浓度(表1).发现南京CO平均质量浓度与广州相当,高于上海(14.3%),低于其他典型城市.南京的工业总产值低于广州和上海,意味着存在污染物输送至南京的情况.南京NO2和SO2平均质量浓度高于北京(69.7%和51.2%)、上海(112.3%和78.1%)、广州(76.6%和80.6%)等一线城市,反映出南京氮氧化物排放较多,工业和汽车尾气排放污染还有待减少.南京PM10平均质量浓度仅高于广州(6.3%),说明扬尘控制较好,PM2.5低于所有参与对比城市.然而南京O3_8h平均质量浓度高于其他典型城市,说明南京已经从颗粒物污染转换成臭氧污染为主的大气复合污染.

  • 2.2 污染时间变化特征

  • 南京市主要大气污染物具有明显的季节变化特征(图3).CO、NO2、SO2、PM10和PM2.5质量浓度均表现出冬高夏低的变化特征.颗粒物冬季污染最为严重(PM10:春(85.3±39.6) μg·m-3,夏 (50.8±23.3) μg·m-3,秋(69.2±39.8) μg·m-3,冬(103.3±54.0) μg·m-3;PM2.5:春(43.5±22.1) μg·m-3,夏(26.7±15.0) μg·m-3,秋(35.1±22.2) μg·m-3,冬(65.8±39.0) μg·m-3).冬季PM10和PM2.5质量浓度均值分别是夏季的2.03和2.46倍,说明南京市细颗粒物的季节变化特征更加显著.粗颗粒物冬季增加,可能是冬季植被覆盖较少地表裸露,易产生扬尘,同时受北方沙尘的输送影响所致;细颗粒物的增加,与冬季边界层较低且层结稳定容易造成颗粒物累积,和周边污染输送相关,这与贾梦唯等[26]结果一致.夏季降雨量大,湿沉降较强,使得大气污染物质量浓度较低.O3_8h则呈现出相反的季节变化趋势,夏季质量浓度高,这是因为太阳辐射增强和日照时间延长,光化学反应加剧有利于臭氧生成[27].本研究期间O3_8h夏季处于较高污染水平(6年夏季平均质量浓度分别为131.3、132.2、135.7、144.4、148.7和122.7 μg·m-3),平均质量浓度是冬季的1.8倍,可以看出O3_8h是夏季重要污染物.

  • 表1 南京与中国其他典型城市大气污染物平均质量浓度对比

  • Table1 Comparison of averaged concentrations of air pollutants between Nanjing and other Chinese cities

  • 参照国家环境质量24h平均二级标准,统计2015—2020年南京市主要污染物超标天数及超标率(图4).本研究期间CO和SO2质量浓度控制较好,没有出现污染超标情况,因此在图4中不再列出.NO2超标天数呈下降趋势,平均减少29.1%.夏季O3_8h质量浓度超标天数占全年超标天数为41.7%~62.0%,成为该季节主要污染物.2015年南京市颗粒物污染最严重,冬季PM10和PM2.5超标天数分别高达34和47d,随后呈现出逐年降低趋势,平均分别降低38.1%和28.1%,至2020年仅有冬季发生颗粒物质量浓度超标事件.通过超标率拟合曲线分析,发现PM10和PM2.5污染下降趋势较为明显(分别降低了38.9%和29.0%),但O3_8h没有明显下降趋势.

  • 图3 2015—2020年南京市主要污染物质量浓度季节变化

  • Fig.3 Seasonal averaged concentration of major air pollutants in Nanjing during2015-2020

  • 图4 2015—2020年南京市主要污染物超标天数及超标率

  • Fig.4 The number of annual pollution days and their ratio for major air pollutants in Nanjing during2015-2020

  • 2.3 污染物空间分布特征

  • 图5显示南京市大气污染物空间分布.CO、NO2和SO2空间分布基本一致,城区(玄武区、秦淮区、建邺区、鼓楼区和雨花台区)大气污染物质量浓度较高,不同季节高值区域变化不大.PM10和PM2.5春夏秋冬四季污染物质量浓度较高区域出现在城区,郊区大气污染物质量浓度较低.主要是因为城市地区人口密度高和交通量大引起机动车排放和家庭排放,产生较多的细颗粒物;同时,市区植被覆盖率较低,易产生扬尘,尤其冬季静稳天气增多不利于扩散造成污染物积累,产生较高的颗粒物浓度,这与前人研究较为一致[28].而郊区人口密集程度和交通拥堵程度低,植被覆盖面积较高,因此颗粒物质量浓度相对较低.对O3_8h而言,春、夏季空间分布较为均一,秋、冬季城区质量浓度低.

  • 2.4 污染物与气象要素相关性分析

  • 表2展示了南京市主要大气污染物与气象要素的皮尔逊相关系数.温度与O3_8h呈显著正相关性(R=0.65,P <0.01),这是因为温度会影响大气湍流和大气化学反应[29],温度较高时大气光化学反应速率加快有利于臭氧生成.相对湿度与大气污染物质量浓度呈负相关关系,跟降水量与大气污染物质量浓度(NO2、SO2、PM10和PM2.5)一致,因为南京发生高相对湿度情况时,一般伴随降水事件,因此湿沉降发生可以去除大气污染物[30-31];另外,降水发生时一般天空覆盖云层,影响太阳辐射抑制臭氧生成,所以呈现负相关性.风速与大气污染物(CO、NO2、SO2、PM10和PM2.5)呈负相关关系,因为风速高有利于大气污染物扩散和传输[32],从而降低污染物质量浓度.颗粒物等污染物质量浓度降低,又能增加大气能见度,增强太阳辐射,有利于臭氧生成,使得风速与O3_8h呈现显著正相关性.

  • 2.5 潜在源分析

  • 从南京市大气污染物季节变化分析,发现冬季时常爆发强度高、持续时间久的大气细颗粒物(PM2.5)重污染事件,而1月是PM2.5质量浓度值最高月份.为了解污染物来源,选取2015—2020年1月,每日24时次的24h后向气团所对应的PM2.5质量浓度分析,质量浓度阈值均设为75 μg·m-3.轨迹计算起始点高度设为500m,研究区域范围选择为(100°~130°E,25°~45°N),网格分辨率为0.5°×0.5°,对南京进行潜在源与PM2.5质量浓度权重分析(图6和图7).结果表明:南京市细颗粒物潜在区分布相对集中,主要来自于南京西南、西和北部,其中WPSCF值大于0.7的地区为安徽地区,WPSCF值在0.6~0.7的地区为江苏北部和山东地区.图7也表明,这些区域对南京市PM2.5的贡献超过75 μg·m-3(高于国家年平均二级标准限值),其中安徽区域的贡献在90 μg·m-3以上.这反映出近年来,随着江苏省(特别是苏南地区)经济的快速发展,江苏省加大排污限制和环境治理,大气环境好于其他省份,所以安徽环境空气污染开始影响江苏;同时,由于冬季植被枯萎地表裸露,北方气团会带来颗粒物污染,江苏北部和山东地区也成为潜在输入源.

  • 2.6 疫情影响

  • 为确定疫情对南京环境空气质量的影响,选取2019—2021年(疫情封控期:2020年1月25日—2月10日)污染物和气象条件进行比较(表3).从温度看,2019、2020、2021年1月25日—2月10日温度分别为4.8、6.1和7.9℃,相差2℃以内.而降水量分别为35.4、 18.6和12.6mm,2019年降水量值最大,但大气污染物数据未表现出明显湿清除情况.2020年相对湿度和风速分别为79.4%和2.5m·s-1,与2019和2021年同期相比相差小于5%,这3年同期时间段,气象要素总体上相差不多.

  • 表2 主要大气污染物质量浓度与气象条件皮尔逊相关系数

  • Table2 Pearson correlation coefficients between major air pollutants and meteorological elements in Nanjing

  • 注:**为0.01水平呈显著相关,*为0.05水平呈显著相关.

  • 图5 大气污染物质量浓度季节空间分布

  • Fig.5 Seasonal spatial distribution of air pollutants in Nanjing

  • 图6 2015—2020年1月南京市PM2.5WPSCF分布

  • Fig.6 WPSCF distribution of PM2.5 in January of 2015-2020in Nanjing

  • 图7 2015—2020年1月南京市PM2.5WCWT分布

  • Fig.7 WCWT distribution of PM2.5 in January of 2015-2020in Nanjing

  • 表3 1月25日—2月10日气象要素对比

  • Table3 Comparison of meteorological elements in Nanjing from Jan.25to Feb.10during2019-2021

  • 从图8可看出,2020年疫情封控期5种大气污染物(CO、NO2、SO2、PM10、PM2.5)质量浓度低于2019年同期,分别降低了10.3%、35.9%、39.0%、38.8%、29.2%,与2021年同期相比,分别降低了24.7%、39.7%、3.0%、41.9%、16.2%.O3_8h在疫情封控期没有下降趋势,分别高于2019和2021年34.7%和31.6%,这可能是由于颗粒物的减少导致太阳辐射增强,促进了臭氧的增加.这说明南京环境空气质量受到了疫情影响[33],因此疫情期间工业停产和交通管制等措施导致人为排放减少,使得部分大气污染物减少.人为排放污染物的减少,可短期内引起气态污染物(CO、NO2、SO2)和颗粒物质量浓度快速下降,但造成O3污染的加重.杭州G20峰会严格管控时期[34]也出现这种情况,说明大气污染物需要科学综合治理,实施联防联控机制.否则,会从一类大气(如颗粒物)污染,转换成另一类大气(臭氧)污染,进而影响治理效果.

  • 3 结论

  • 1)研究期间,CO、NO2、SO2、O3_8h、PM10和PM2.5平均质量浓度分别为800、43.1、13.0、106.0、77.1和43.0 μg·m-3.与中国典型城市(北京、上海、广州、成都、兰州和武汉)相比,南京PM2.5平均质量浓度最低,而O3_8h平均质量浓度高于其他城市.

  • 2)2015—2020年南京NO2、PM10和PM2.5超标天数呈下降趋势,平均减少率分别为29.1%、38.1%和28.1%,而臭氧超标天数呈上升趋势.臭氧质量浓度夏季最高,平均值为135.8 μg·m-3,而其他5种污染物(CO、NO2、SO2、PM10和PM2.5)冬季质量浓度最高,平均值分别为1 000、52.3、15.9、104.2和67.2 μg·m-3.

  • 3)2015—2020年1月南京地区细颗粒物潜在源区分布相对集中,主要潜在源来自安徽省,WPSCF值大于0.7,江苏北部和山东地区WPSCF值在0.6~0.7.在1月大气污染物输送影响着南京环境空气质量.

  • 4)在气象条件类似的状态下,与2019年和2021年同期相比,2020年疫情封控期大气污染物(CO、NO2、SO2、PM10和PM2.5)质量浓度最低,说明疫情封控措施对南京环境空气质量产生显著影响.

  • 图8 2020年疫情封控前后污染物质量浓度与前后年份同期对比

  • Fig.8 Daily concentrations of air pollutants around Jan.25from 2019to 2021

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