夏季长三角地区臭氧非线性响应曲面模型的建立及应用23501.pdf

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1、36420164Acta Scientiae CircumstantiaeVol 36 No 4Apr2016No 2014BAC22B03No14DZ1202905No2014-01Supported by the National Key Technology D ProgramNo 2014BAC22B03the Scientific and Technological Project of Shanghai Science andTechnology Committee No 14DZ1202905and the Key Project of Shanghai Environmenta

2、l Protection Bureau Shanghai Branch No 2014-011988E-mail yanrs saes sh cn*E-mail lili saes sh cnBiographyYAN usha 1988femaleE-mail yanrs saes sh cn*Corresponding author E-mail lili saes sh cnDOI 10 13671/j hjkxxb2015 0678 2016J 36 41383-1392Yan SLi LAn J Yet al 2016 Establishment and application of

3、nonlinear response surface model of ozone in the Yangtze iver Delta region duringsummertime J Acta Scientiae Circumstantiae 36 41383-1392121 2*1 21 21 234Carey J Jang5Joshua S Fu612002332200233310008445100065 Air Quality Modeling GroupOffice of Air Quality Planning and StandardsU S Environmental Pro

4、tection AgencyNC 27711USA6 Civil and Environmental EngineeringUniversity of TennesseeKnoxvilleTN37996 USA2015-03-302015-09-272015-10-0720138WF-CMAQesponse surface modelingSM SMO3O3O3O3O3、VOC、NOx O3O3NOxO350%O372 1%27 9%11070%20138O3CMAQ0253-2468 2016 04-1383-10X515AEstablishment and application of n

5、onlinear response surface model of ozone inthe Yangtze iver Delta region during summertimeYAN usha1 2LI Li1 2*AN Jingyu1 2LU Qing1 2HUANG Cheng1 2WANG Shuxiao3ZHU Yun4Carey J Jang5Joshua S Fu61 State Environmental Protection Key Laboratory of the Cause and Prevention of Urban Air Pollution ComplexSh

6、anghai 2002332 Shanghai Academy of Environmental SciencesShanghai 2002333 School of EnvironmentTsinghua UniversityBeijing 1000844 College of Environment and EnergySouth China University of TechnologyGuangzhou 5100065 Air Quality Modeling GroupOffice of Air Quality Planning and StandardsU S Environme

7、ntal Protection AgencyNC 27711USA6 Civil and Environmental EngineeringUniversity of TennesseeKnoxvilleTN37996 USAeceived 30 March 2015received in revised form 27 September 2015accepted 7 October 2015AbstractA large-scale ozone pollution episode occurred in early August 2013 in the Yangtze iver Delta

8、 region In this paperthe response surface36modelSMwas employed to build the functional relationships between ozone precursorsNOxand VOCemissions and ozone concentration based onWF-CMAQ air quality model and emission inventories of anthropogenic air pollutants in the Yangtze iver Delta region Sensiti

9、vity characteristics ofozone chemistrysource contributions of ozone and variations of ozone concentrations under different scenarios were analyzedand the optimal controlscheme based on case study was proposed The dominant control factors for ozone pollution showed clear regional differences in the Y

10、angtze iver Deltaregion The urban sites such as Shanghai Academy of Environmental SciencesHangzhou Wolong Bridge and Nanjing Xuanwu Lake were VOC-limitedwhile the rural areas such as Xuzhou TongshanHefei FeixiLishui Qingtian were NOx-limited The sensitivity characteristics of ozone were dependent on

11、its concentrations With the increase of ozone concentrationall areas presented higher sensitivity to NOx The long-distance transport contributed morethan 50%of ozone pollution in Shanghai on usual days During pollution episodeslocal and regional sources contributed 72 1%whilelong-distancetransport c

12、ontribution decreased to 27 9%By estimating ozone concentrations for 110 groups of scenarios by SMwe concluded that ozone concentrationwould achieve attainment if the emission of ozone precursors from both local and regional sources were reduced by 70%in August 2013 in ShanghaiKeywordsozoneresponse

13、surface model SMCMAQYD egion1IntroductionNOxVOCFannet al2012Brandt et al2013Adon et al2013 Sillman et al2009Li et al20122009 O3NOxVOCO3O3O3O3Chou et al2011、DDMItahashi et al2012OSATLi et al2012 O3/NOz、HCHO/NOy、H2O2/HNO3O3Liu et al2010 DDM、Yarwoodet al2013Tang et al2014 Soontae2009CMAQHDDMDallas Fort

14、 WorthNOxVOCsNOxDDMDunker et al2002 OSATO3 Li2013、2014OSAT、O3O3Wang et al2009 SMWang et al201120138O3、O32Model and parameters2 1SMWF-CMAQO3NOxVOCO3、O3、O32 2WFv3 4 148314CMAQv5 0CMAQCB05 Yarwood et al2005D0136 km 36 kmD0212 km 12 kmD034 km4 km1D01D02Zhang20092006INTEX-BD03Huang et al2011Li et al 2011

15、201381Fig 1Sketch map of modeling domainSM、O3NOxVOCNOxVOCLHSLatin HypercubeSampleStein 1987Xing et al2011NOxVOCSM203020 1 5 SMO32LHSFig 2Sampling results based on LHS method2 3SMCMAQ、SM、SMSMSMSMCMAQSMCMAQSMCMAQCMAQ Xing2011SMSM23 120138、4CMAQ3O3CMAQ4O325831360 520 660 41、034 3O3abcdFig 3Comparison o

16、f modeled and monitored O3concentration23 24301300 12 ppb1 08 ppb6%SM-O31Table 1Evaluation indicators of leave-one-out cross validation0 122 132 501 080 332 790 13%3 74%4 97%1 69%0 50%5 51%0 03%3 97%4 59%1 81%0 59%5 39%ppb2 3 34SM-O3Fig 4esults of leave-one-out cross validation66CMAQ6SM560 920 5%SM-

17、O3683145Fig 5esults of out-of-sample validation2Table 2Evaluation indicators of out-of-sample validation0 160 560 060 270 060 610 23%0 76%0 09%0 41%0 10%0 82%0 24%0 77%0 08%0 41%0 10%0 83%ppb3esults3 1SMO3O3NOxVOCVOCVOC1O3NOxO3PPeak atio PNOxNOxO3O3VOCPNOxNOxO3O3NOx PO3O3NOxVOCPNOxNOxNOxXing et al20

18、11 PSM3 1 1NOxVOCP、6、3、NOxP0 68、0 97、0 971VOCNOxO373NOxP1NOxNOxO37831366NOxVOCO3abcFig 6esponse relationship between emission variations of NOxVOC and O3concentrations in urban zones of the YD egion7NOxVOCO3a-b-c-Fig 7esponse relationship between emission variations of NOxVOC and O3concentrations in

19、 rural zones of the YD egion883143 1 2O3100 ppb、60 100 ppb、40 60 ppb、3PO383PO30 930 68048P、31 13、0 72、0 63P、31 01、0 72、0 54O3NOxO3NOx8O3100 ppb、60 100 ppb、40 60 ppbNOxVOCO3abcFig 8esponse relationship between emission variations of NOxVOC and O3concentrations at high over 100 ppbmedium 60 100 ppblow

20、40 60 ppbO3concentration3 2O3O3O3SM-O3NOxVOCO3O39a20138O351 3%O3VOC17 2%NOx2 5%29 0%18 9%NOx10 1%VOCO310O3510O310983136O327 9%33 7%38 4%O39O3abFig 9Monthly mean of daily 1 h maxima O3concentrationaand O3concentration on pollution daysbin Shanghai10O3Fig 10Diurnal variation of daily 1 h maxima O3conc

21、entration in ShanghaiO3O3SM-O3110O320138O3O3200 gm3100 ppb0 1 5SMNOxVOCO3O3O3O311a110100O3O3O3O3O3811b59c5950%、90%、6009314c6060%、100%、68c68、77c77、87c8797c976NOxVOC c59c60c87c97c6860%、80%c7770%c77O370%O311O3aO3bFig 11Scenarios design for O3attainmentaand O3concentration prediction of attained scenari

22、osb2015O38h42 79%10 17%28 94%8 49%20142013O361 2%22 8%O351 3%19 7%、O38 h、O3、O3、CAMxOSAT、CMAQSMD01D022006INTEX-B2013O3O380 ppb30%70%Li et al 2012O327 9%72 1%Zhang2011O320%50%O3O3O34Conclusions1SM-O3O32O3、VOC、NOxO3O3NOx320138O350%19 7%29 0%O3100 ppb27 9%72 1%4O370%20131931368O3eferencesAdon M Galy-Lac

23、aux C Delon C et al 2013 Dry deposition of nitrogencompoundsNO2HNO3NH3sulfur dioxide and ozone in westand central African ecosystems using the inferential methodJ Atmospheric Chemistry and Physics 13 2211351-11374Brandt J Silver J D Christensen J H et al 2013 Contribution from theten major emission

24、sectors in Europe and Denmark to the health-costexternalities of air pollution using the EVA model system-anintegrated modelling approachJ Atmospheric Chemistry andPhysics 13 157725-7746Chou C C K Tsai C Y Chang C C et al 2011 Photochemical productionof ozone in Beijing during the 2008Olympic GamesJ

25、Atmospheric Chemistry and Physics 11 189825-9837Dunker A M Yarwood G Ortmann J P et al 2002 Comparison of sourceapportionment and source sensitivity of ozone in a three-dimensionalair quality modelJ Environmental Science Technology 36132953-2964Fann N Lamson A D Anenberg S C et al 2012 Estimating th

26、e nationalpublic health burden associated with exposure to ambient PM2 5andozone J isk Analysis 32 181-95Huang CChenCHLiLet al 2011 Emissioninventoryofanthropogenic air pollutants and VOC species in the Yangtze iverDelta region ChinaJ Atmospheric Chemistry and Physics 114105-4120Itahashi S Uno I Kim

27、 S 2012 Source contributions of sulfate aerosol overEast Asia estimated by CMAQ-DDM J Environmental Science Technology 46 126733-6741 2015 2013O3J 36 11-10Li L Chen C Huang C et al 2011 Ozone sensitivity analysis with theMM5-CMAQ modelingsystemforShanghaiJ JournalofEnvironmental Sciences 23 71150-11

28、57Li L Chen C H Fu J S et al 2011 Air quality and emissions in theYangtze iver DeltaChinaJ Atmospheric Chemistry andPhysics 11 1621-1639Li Y Lau A Fung J et al 2012 Ozone Source ApportionmentOSATto differentiate local regional and super regional source contributionsin the Pearl iver Delta region Chi

29、naJ Journal of Geophysicsesearch 117 D15DOI10 1029/2011JD017340Li Y Lau A K H Fung J C H et al 2013 Systematic evaluation of ozonecontrol policies using an Ozone Source Apportionment method J Atmospheric Environment 76136-146Liu X H Zhang Y Xing J et al 2010 Understanding of regional airpollution ov

30、er China using CMAQ-Part II Process analysis andozonesensitivitytoprecursoremissionsJAtmosphericEnvironment 44 203719-3727Sillman S West J J 2009 eactive nitrogen in Mexico City and itsrelation to ozone-precursor sensitivityresults from photochemicalmodelsJ AtmosphericChemistryandPhysics9113477-3489

31、Soontae K Daewon W Byuna D C 2009 Contributions of inter-andintra-state emissions to ozone over Dallas-Fort Worth TexasJ Civil Engineering and Environmental Systems 70 103-116Stein M 1987 Large sample properties of simulations using Latinhypercube sampling J Technometrics 29 2143-151Tang W Cohan D S

32、 Pour-Biazar A et al 2014 Influence of satellite-derived photolysis rates and NOxemissions on Texas ozone modelingJ Atmospheric Chemistry and Physics Discussions 141724475-24522Van Loon M Vautard Schaap M et al 2007 Evaluation of long-termozone simulations from seven regional air quality models and

33、theirensemble J Atmospheric Environment 41 102083-2097Wang S Xing J Jang C et al 2011 Impact assessment of ammoniaemissions on inorganic aerosols in East China using response surfacemodeling technique J Environmental Science and Technology 45219293-9300 2009J B39 6548-559 2014OSAT2010J 343567-573Wan

34、g Z S Chien C J Tonnesen G S 2009 Development of a taggedspecies source apportionment Algorithm to characterize three-dimensionaltransportandtransformationofprecursorsandsecondary pollutantsJ JournalofGeophysicalesearchAtmospheres1984-2012114 D216149-6150Xing J Wang S X Jang C et al 2011 Nonlinear r

35、esponse of ozone toprecursor emission changes in Chinaa modeling study usingresponse surface methodologyJ Atmospheric Chemistry andPhysics 11 105027-5044Yarwood G ao S Yocke M et al 2005 Updates to the Carbon BondMechanismCB05 T-04-00675 DurhamNC US EPAYarwood G Emery C Jung J et al 2013 A method to

36、 represent ozoneresponse to large changes in precursor emissions using high-ordersensitivity analysis in photochemical modelsJ GeoscientificModel Development 6 51601-1608Zhang Q Streets D G Carmichael G et al 2009 Asian emissions in2006 for the NASA INTEX-B mission J Atmospheric Chemistryand Physics 9 145131-51532931

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