A monitoring-modeling approach to SO_4~(2-) and NO_3~- secondary conversion ratio estimation during haze periods in Beijing, China
详细信息    查看全文 | 推荐本文 |
  • 英文篇名:A monitoring-modeling approach to SO_4~(2-) and NO_3~- secondary conversion ratio estimation during haze periods in Beijing, China
  • 作者:Xiaoqi ; Wang ; Wei ; Wei ; Shuiyuan ; Cheng ; Chong ; Zhang ; Wenjiao ; Duan
  • 英文作者:Xiaoqi Wang;Wei Wei;Shuiyuan Cheng;Chong Zhang;Wenjiao Duan;Key Laboratory of Beijing on Regional Air Pollution Control,Beijing University of Technology;Collaborative Innovation Center of Beijing City Traffic,Beijing University of Technology;
  • 英文关键词:Haze periods;;SO_4~(2-) and NO_3~-;;Secondary conversion;;Secondary oxidation ratio
  • 中文刊名:HJKB
  • 英文刊名:环境科学学报(英文版)
  • 机构:Key Laboratory of Beijing on Regional Air Pollution Control,Beijing University of Technology;Collaborative Innovation Center of Beijing City Traffic,Beijing University of Technology;
  • 出版日期:2019-03-08
  • 出版单位:Journal of Environmental Sciences
  • 年:2019
  • 期:v.78
  • 基金:supported by the National Key R&D Program of China (No. 2016YFC0202705);; the National Natural Science Foundation of China (Nos. 51638001 and 51478017);; the funding support from Beijing Municipal Commission of Science and Technology (Nos. Z161100004516013 and Z171100002217002)
  • 语种:英文;
  • 页:HJKB201904028
  • 页数:10
  • CN:04
  • ISSN:11-2629/X
  • 分类号:295-304
摘要
SO_4~(2-) and NO_3~- are important chemical components of fine particulate matter(PM_(2.5)),especially during haze periods.This study selected two haze episodes in Beijing,China with similar meteorological conditions.A monitoring-modeling approach was developed to estimate the secondary conversion ratios of sulfur and nitrogen based on monitored and simulated concentrations.Measurements showed that in Episode 1(24th–25th October,2014),the concentrations(proportions)of SO_4~(2-) and NO_3~- reached 35.1μg/m~3(14.9%) and 55.0μg/m~3(22.9%),while they reached 14.4μg/m~3(9.3%) and 59.1μg/m~3(38.1%)in Episode 2(26th–27th October,2017).A modeling system was applied to apportion Beijing's SO_4~(2-) and NO_3~- in primary and secondary SO_4~(2-)/NO_3~- emitted from local and regional sources.Thus,secondary conversion contributions considering the local and regional level were defined.The former primarily focused on Beijing atmospheric oxidation ability and the latter mainly considered the existence form of Beijing SO_4~(2-)/NO_3~- under the regional transport impacts.Finally,secondary oxidation ratios were estimated through combining secondary conversion contribution coefficients for simulated and monitored concentrations.At regional level,sulfur oxidation ratios in polluted(clean)days during two sampling periods were0.57–0.72(0.07–0.52)and 0.74–0.80(0.08–0.61),nitrogen oxidation ratios were 0.20–0.29(0.05–0.15)and 0.34–0.38(0.02–0.29),indicating that atmospheric oxidation was enhanced when considering regional transport through 2014–2017.At the local level,sulfur oxidation ratios were 0.66–0.71(0.04–0.48)in haze(clean)days,while nitrogen oxidation ratios were0.16–0.29(0.02–0.16).The atmospheric oxidation ability markedly increased in PM_(2.5)pollution days,but changed only slightly between the two periods.
        SO_4~(2-) and NO_3~- are important chemical components of fine particulate matter(PM_(2.5)),especially during haze periods.This study selected two haze episodes in Beijing,China with similar meteorological conditions.A monitoring-modeling approach was developed to estimate the secondary conversion ratios of sulfur and nitrogen based on monitored and simulated concentrations.Measurements showed that in Episode 1(24th–25th October,2014),the concentrations(proportions)of SO_4~(2-) and NO_3~- reached 35.1μg/m~3(14.9%) and 55.0μg/m~3(22.9%),while they reached 14.4μg/m~3(9.3%) and 59.1μg/m~3(38.1%)in Episode 2(26th–27th October,2017).A modeling system was applied to apportion Beijing's SO_4~(2-) and NO_3~- in primary and secondary SO_4~(2-)/NO_3~- emitted from local and regional sources.Thus,secondary conversion contributions considering the local and regional level were defined.The former primarily focused on Beijing atmospheric oxidation ability and the latter mainly considered the existence form of Beijing SO_4~(2-)/NO_3~- under the regional transport impacts.Finally,secondary oxidation ratios were estimated through combining secondary conversion contribution coefficients for simulated and monitored concentrations.At regional level,sulfur oxidation ratios in polluted(clean)days during two sampling periods were0.57–0.72(0.07–0.52)and 0.74–0.80(0.08–0.61),nitrogen oxidation ratios were 0.20–0.29(0.05–0.15)and 0.34–0.38(0.02–0.29),indicating that atmospheric oxidation was enhanced when considering regional transport through 2014–2017.At the local level,sulfur oxidation ratios were 0.66–0.71(0.04–0.48)in haze(clean)days,while nitrogen oxidation ratios were0.16–0.29(0.02–0.16).The atmospheric oxidation ability markedly increased in PM_(2.5)pollution days,but changed only slightly between the two periods.
引文
BJEPB(Beijing Environmental Protection Bureau),2014.Beijing Environmental Statement 2013.Available.http://www.bjstats.gov.cn/tjsj/tjgb/ndgb/201511/t20151124_327761.html,Accessed date:28 October 2018.
    BJEPB(Beijing Environmental Protection Bureau),2015.Beijing Environmental Statement 2014.Available.http://www.bjstats.gov.cn/tjsj/tjgb/ndgb/201511/t20151124_327764.html,Accessed date:28 October 2018.
    BJEPB(Beijing Environmental Protection Bureau),2018.Beijing Environmental Statement 2017.Available.http://www.bjstats.gov.cn/tjsj/tjgb/ndgb/201803/P020180302397365111421.pdf,Accessed date:28 October 2018.
    Gao,X.,Yang,L.,Cheng,S.,Gao,R.,Zhou,Y.,Xue,L.,et al.,2011.Semi-continuous measurement of water-soluble ions in PM2.5in Jinan,China:Temporal variations and source apportionments.Atmos.Environ.45(33),6048-6056.
    Gao,J.,Tian,H.,Cheng,K.,Lu,L.,Zheng,M.,Wang,S.,et al.,2015.The variation of chemical characteristics of PM2.5,and PM10,and formation causes during two haze pollution events in urban Beijing,China.Atmos.Environ.107,1-8.
    Gao,J.,Wang,K.,Wang,Y.,Liu,S.,Zhu,C.,Hao,J.,et al.,2017.Temporal-spatial characteristics and source apportionment of PM2.5as well as its associated chemical species in the BeijingTianjin-Hebei region of China.Environ.Pollut.233,714.
    Guo,Y.,Gao,X.,Zhu,T.,Luo,L.,Zheng,Y.,2017.Chemical profiles of PM emitted from the iron and steel industry in northern China.Atmos.Environ.150,187-197.
    He,K.,Yang,F.,Ma,Y.,Zhang,Q.,Yao,X.,Chan,C.K.,et al.,2001.The characteristics of PM2.5in Beijing,China.Atmos.Environ.35(29),4959-4970.
    He,H.,Wang,Y.,Ma,Q.,Ma,J.,Chu,B.,Ji,D.,et al.,2014.Mineral dust and NOx promote the conversion of SO2to sulfate in heavy pollution days.Sci.Rep.4(1),4172.
    Hu,G.,Zhang,Y.,Sun,J.,Zhang,L.,Shen,X.,Lin,W.,et al.,2014.Variability,formation and acidity of water-soluble ions in PM2.5,in Beijing based on the semi-continuous observations.Atmos.Res.145-146,1-11.
    Huang,X.,Liu,Z.,Zhang,J.,Wen,T.,Ji,D.,Wang,Y.,2016.Seasonal variation and secondary formation of size-segregated aerosol water-soluble inorganic ions during pollution episodes in Beijing.Atmos.Res.168,70-79.
    Ji,D.,Li,L.,Wang,Y.,Zhang,J.,Cheng,M.,Sun,Y.,et al.,2014.The heaviest particulate air-pollution episodes occurred in northern China in January,2013:Insights gained from observation.Atmos.Environ.92,546-556.
    Jia,J.,Cheng,S.,Yao,S.,Xu,T.,Zhang,T.,Ma,Y.,et al.,2018.Emission characteristics and chemical components of sizesegregated particulate matter in iron and steel industry.Atmos.Environ.182,115-127.
    Lang,J.,Cheng,S.,Wei,W.,Zhou,Y.,Wei,X.,Chen,D.,2012.Astudy on the trends of vehicular emissions in the BeijingTianjin-Hebei(BTH)region,China.Atmos.Environ.62(15),605-614.
    Lang,J.,Cheng,S.,Li,J.,Chen,D.,Zhou,Y.,Wei,X.,et al.,2013.Amonitoring and modeling study to investigate regional transport and characteristics of PM2.5pollution.Aerosol Air Qual.Res.13(3),943-956.
    Lang,J.,Zhang,Y.,Zhou,Y.,Cheng,S.,Chen,D.,Guo,X.,et al.,2017.Trends of PM2.5and chemical composition in Beijing,2000-2015.Aerosol Air Qual.Res.17(2),412-425.
    Leoni,C.,Pokorná,P.,Hovorka,J.,Masiol,M.,Topinka,J.,Zhao,Y.,et al.,2018.Source apportionment of aerosol particles at a European air pollution hot spot using particle number size distributions and chemical composition.Environ.Pollut.234,145-154.
    Li,X.,Wang,L.,Ji,D.,Wen,T.,Pan,Y.,Sun,Y.,et al.,2013.Characterization of the size-segregated water-soluble inorganic ions in the Jing-Jin-Ji urban agglomeration:spatial/temporal variability,size distribution and sources.Atmos.Environ.77(7),250-259.
    Li,Z.,Jiang,J.,Ma,Z.,Wang,S.,Duan,L.,2015.Effect of selective catalytic reduction(SCR)on fine particle emission from two coal-fired power plants in China.Atmos.Environ.120,227-233.
    Li,J.,Qi,Z.,Li,M.,Wu,D.,Zhou,C.,Lu,S.,et al.,2017.Physical and chemical characteristics of condensable particulate matter from an ultralow-emission coal-fired power plant.Energ.Fuels31(2),1778-1785.
    Lv,B.,Zhang,B.,Bai,Y.,2016.A systematic analysis of PM2.5,in Beijing and its Sources from 2000 to 2012.Atmos.Environ.124,98-108.
    Ma,J.,Chu,B.,Liu,J.,Liu,Y.,Zhang,H.,He,H.,2017.NOx promotion of SO2conversion to sulfate:an important mechanism for the occurrence of heavy haze during winter in Beijing.Environ.Pollut.233,662-669.
    Meng,C.,Wang,L.,Zhang,F.,Wei,Z.,Ma,S.,Ma,X.,et al.,2016.Characteristics of concentrations and water-soluble inorganic ions in PM2.5,in Handan city,Hebei province,China.Atmos.Res.171,133-146.
    Meng,Z.,Lin,W.,Zhang,R.,Han,Z.,Jia,X.,2017.Summertime ambient ammonia and its effects on ammonium aerosol in urban Beijing,China.Sci.Total Environ.579,1521-1530.
    Ping,X.,Zhou,X.,Duan,J.,Tan,J.,He,K.,Yuan,C.,et al.,2017.Chemical characteristics of water-soluble organic compounds(WSOC)in PM2.5,in Beijing,China:2011-2012.Atmos.Res.183,104-112.
    Saarnio,K.,Frey,A.,Niemi,J.V.,Timonen,H.,Ronkko,T.,Karjalainen,P.,et al.,2014.Chemical composition and size of particles in emissions of a coal-fired power plant with flue gas desulfurization.J.Aerosol Sci.73(12),14-26.
    Sun,Y.,Zhuang,G.,Tang,A.,Wang,Y.,An,Z.,2006.Chemical characteristics of PM2.5and PM10in haze-fog episodes in Beijing.Environ.Sci.Technol.40(10),3148-3155 2006.
    Sun,Y.,Wang,Z.,Du,W.,Zhang,Q.,Wang,Q.,Fu,P.,et al.,2015.Long-termreal-time measurements of aerosol particle composition in Beijing,China:Seasonal variations,meteorological effects,and source analysis.Atmos.Chem.Phys.15(17),10149-10165.
    Wang,G.,2017.Verification of air pollution sources inventory in the Beijing-Tianjin-Hebei region and the study of new technology optimal reduction and demonstration application.PhDthesis.Beijing University of Technology,Beijing,China.
    Wang,Y.,Zhuang,G.,Tang,A.,Yuan,H.,Sun,Y.,Chen,S.,et al.,2005.The ion chemistry and the source of PM2.5aerosol in Beijing.Atmos.Environ.39(21),3771-3784.
    Wang,H.,Xu,J.,Zhang,M.,Yang,Y.,Shen,X.,Wang,Y.,et al.,2014.A study of the meteorological causes of a prolonged and severe haze episode in January 2013 over Central-Eastern China.Atmos.Environ.98(98),146-157.
    Wang,X.,Lang,J.,Cheng,S.,Chen,G.,Liu,X.,2016a.Study on transportation of PM2.5in Beijing-Tianjin-Hebei(BTH)and its surrounding area.China Environ.Sci.36(11),3211-3217.
    Wang,Z.,Zhang,D.,Li,Y.,Dong,X.,Sun,R.,Sun,N.,2016b.Different air pollution situations of O3and PM2.5during summer in Beijing.Environ.Sci.3(9),807-815.
    Wang,G.,Cheng,S.,Lang,J.,Yang,X.,Wang,X.,Chen,G.,et al.,2017.Characteristics of PM2.5and assessing effects of emission-reduction measures in the heavy polluted city of Shijiazhuang,before,during,and after the Ceremonial Parade2015.Aerosol Air Qual.Res.17(2),499-512.
    Wen,W.,Ma,X.,Wei,P.,Cheng,S.,Wang,X.,2018.Understanding the regional transport contributions of primary and secondary PM2.5components over Beijing during a severe pollution episodes.Aerosol Air Qual.Res.18(7),1720-1733.
    Xue,W.,Fei,F.,Wang,J.,Tang,G.,Yu,L.,Yang,J.,et al.,2014.Numerical study on the characteristics of regional transport of PM2.5in China.China Environ.Sci.34(6),1361-1368.
    Yan,J.,Bao,J.,Yang,L.,Fan,F.,Shen,X.,2011.The formation and removal characteristics of aerosols in ammonia-based wet flue gas desulfurization.J.Aerosol Sci.42(9),604-614.
    Yang,Y.,Zhou,R.,Wu,J.,Yu,Y.,Ma,Z.,Zhang,L.,et al.,2015.Seasonal variations and size distributions of water-soluble ions in atmospheric aerosols in Beijing,2012.J.Environ.Sci.34(8),197-205.
    Yang,X.,Cheng,S.,Li,J.,Lang,J.,Wang,G.,2017.Characterization of chemical composition in PM2.5in Beijing before,during,and after a large-scale international event.Aerosol Air Qual.Res.17(4),896-907.
    Yao,S.,Cheng,S.,Li,J.,Zhang,H.,Jia,J.,Sun,X.,2018.Effect of wet flue gas desulfurization(WFGD)on fine particle(PM2.5)emission from coal-fired boilers.J.Environ.Sci.https://doi.org/10.1016/j.jes.2018.05.005.
    Zhao,P.,Xu,X.,Meng,W.,Dong,F.,He,D.,Shi,Q.,et al.,2012.Characteristics of hazy days in the region of Beijing,Tianjin,and Hebei.China Environ.Sci.32(1),31-36.
    Zhou,Y.,2012.Study and application of regional atmospheric pollutants emission inventories development and sensitive emission sources identification.PhD thesis.Beijing University of Technology,Beijing,China.
    Zhou,Y.,Cheng,S.,Li,J.,Lang,J.,Li,L.,Chen,D.,2012.A new statistical modeling and optimization framework for establishing high-resolution PM10,emission inventory-II.Integrated air quality simulation and optimization for performance improvement.Atmos.Environ.60(1),623-631.

© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号

地址:北京市海淀区学院路29号 邮编:100083

电话:办公室:(+86 10)66554848;文献借阅、咨询服务、科技查新:66554700