大気浮遊粒子の発生源推定

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こうだいひきぎ
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1 Source Apportionment of Suspended Particulate Matter Masayoshi Karasawa, Hitoshi Mizuta, Yuzo Kawai, Hiroshi Ito, Takeshi Kogiso SPM CEB FA ' SPM Cae Na Al K Fe V Zn CEB SPM 4 CEB A chemical element balance (CEB) method and a factor analysis (FA) method were used to estimate the contributions of particle sources to ambient suspended particulate matters (SPM). The SPM samples were simultaneously collected at four sites around Nagoya City in November and December, Elements and ions were analyzed using an organic element analyzer, ICP-AES, AAS and ion chromatography. The contributions of six major sources ( soil, sea salt, heavy oil combustion, iron and steel industry, refuse incineration and diesel engine ) and secondary particles were calculated by the CEB method using seven elements of elemental carbon, Na, Al, K, V, Fe and Zn. Nearly 75% of the SPM can be accounted for by primary and secondary aerosols. The contributions of diesel engine, secondary particles and soil were considerably large. On the other hand, those of iron and steel industry, heavy oil combustion and refuse incineration were less than 5%. On factor analysis of the data of 16 samples for 15 chemical components, four factors were identified. These factors were associated with not only source types but also weather conditions and regional features. Therefore, it is necessary to take this fact into consideration in estimating source contributions from the absolute factor score. However, the FA method is very useful in determining the source apportionment of the SPM in the area with no source profile data. Since precision of the source contributions calculated using the CEB method depends on the reliability of the data of source emission composition, it is extremely important to accumulate the source data. ( SPM ) ICP-AES R&D Vol. 29 No. 2 ( )

2 ( 10µm : SPM ) 50 NO 2 SPM source-receptor relationships SO 2 source receptor source SPM SPM source-receptor relationships receptor SPM receptor receptor SPM CEB receptor SPMCEB 4 SPM NO X SO 2 NO X SO 2 SPMsource SPMNO X SO NO X 89 3 Methods to analyze source-receptor relationship. 701m 19 27m m 5km R&D Vol. 29 No. 2 ( )

Fig. 2 H Fig. 2 F 10µm HVS-1000 2 Fig. 3 6003 QR- 100 8in 10in ADVANTEC SPM SPM 11 12 4 48 4 0:00 24:00 Fig.

4 Photograph of Mikuniyama site. Sampling points and location of major sources.

Sites Mean value Population Manufacture Distance of NO X density production from a coast Mikuniyama 159 1.

3 Fig. 2 H Fig. 2 F 10µm HVS Fig QR in 10in ADVANTEC SPM SPM :00 24:00 Fig. 2 1 SPM C H N CHN 240C SPM Fig. 42 SPM Ct N Cae Cao CtCae Fig. 4 Photograph of Mikuniyama site. Sampling points and location of major sources. : Nagoya meteorological observatory Some features of four sites. Sites Mean value Population Manufacture Distance of NO X density production from a coast Mikuniyama Kasugai Nagoya Chita ppb n/km 2 yen/km 2 km Partition of the quartz filter and chemical analysis methods. R&D Vol. 29 No. 2 ( )

4 ICPS-2000 Mg Al Ca Ti V Ni Zn Pb SAS7500 Na K Na K Ca Al Mg Fig ml µm 4020i DIONEX NH 4 Cl NO 3 SO 2 4 SO 2 4 CEB 100 F j (1) χ 2 = (C i A i j F j ) 2 2 / C i i j C i SPMi A i j j i SPM SPMCae SPM 2 Cae SPM µm Source profile data used in CEB method ( unit: % ) Soil Sea salt Heavy oil g Iron e Refuse d Diesel a A i j η A i j η A i j η A i j η A i j η A i j η Cae b c Cao b c Na Mg 0.43 nr nr nr nr nr Al Cl K Ca Ti < V < Fe Ni < Zn < Pb < NO 3 SO nr 0.2 c b f f f c b 3.0 nr: no report, a: ref 9), b: ref. 13), c: ref. 14), d: ref. 11), e: ref. 12), f: ref. 15), g: ref. 10) R&D Vol. 29 No. 2 ( )

5 V A B C Cae CaoSO 2 4 η (2)Table 2 η i j = 100 A i j / j A i j ηceb Al Na VFe Zn K Cae7 Cao η NO 3 SO 2 4 Cao NO 3 SO 2 4 Cao [ ] R [ ] P [ ] S (3) 2 2 [SPM] S 132/96 { [SO 4 ] R [SO 4 ] P } + 80/62 { [NO 3 ] R [NO 3 ] P } + [Cao] R [Cao] P (3) i CEB [C i ] P = M 0 A i j F j j M 0 SPM SPM SPM i n { X α i α 1 n i 1 p } X i σ i Z α i X α i Xi σ i E Z α i 1 Z fa t E a f α Minres b f (6) Z f b t E 01 µg m 3 Thurston Ito Z f α j β 1 j Z α 1 + β 2 j Z α 2 + +β p j Z α n (8) 0 0 Z 0 i 0 X i / σ i Z 0 i(8)denormalization constants' f 0 j f 0 j β 1 j Z β 2 j Z β p j Z 0 p f α j f α j f α j f 0 j 0 SPM M α f α j 'mass scaling factors' q j R&D Vol. 29 No. 2 ( )

6 M α q 0 q 1 f α 1 q 2 f α 2 q m f α m α j q j f α j 4 4 RUN 1 3 RUN RUN 1 100µg m 3 RUN RUN 3 RUN RUN µg m 3 700m RUN 1 Sampling period and weather conditions. NO Period W (m/s) RH (%) RUN 1 ' (Sun.) RUN 2 ' (Wed.) RUN 3 ' (Sun.) RUN 4 ' (Wed.) W: Wind speed, RH: Relative humidity. Distribution of SPM concentration. Weather charts of each sampling days. R&D Vol. 29 No. 2 ( )

7 SPM RUN 1 RUN m Na RUN 3 Na Table 2 AlRUN 2 RUN 2 Al 4mm Fe V SPM NH 4 NO 3 Cl SO 2 4 NO 3 SO 2 4 SO 2 4 NO 3 7 Cae Na Al K Fe V Zn CEB 6 L/S Large/Small 7 L/S1.1 NH 4 Cl Mg Cl HCl Cl Table 2 Cao NH 4 L/S Concentration of main components. R&D Vol. 29 No. 2 ( )

8 Chemical element balance of Nagoya aerosol on RUN 2. Chemical element balances of SPM Sample No: Nagoya Contributions [ ng/m 3 ] Total conc. [ ng/m 3 ] Element Soil Sea salt Heavy oil Iron Refuse Diesel Second Calculated Observed L/S PM Tracer Cae Na Al K V Fe Zn Other Cao Mg Ca Ti Ni Pb Cl NO SO NH 4 + CEB RUN RUN 1 RUN 2 RUN mm/ RUN 3 RUN 3 CEB Soil Sea salt Sampling point Mikuniyama Kasugai Nagoya Chita Source contributions of each samplings by the CEB method. R&D Vol. 29 No. 2 ( )

9 4 Four hour periodic changes of wind direction and speed at Nagoya meteorological observatory. 5µg/m 3 1/ Ni Ti 15SPM Cae Cao K NO 3 NH + 4 K (a)f1 F2 F4 Average contributions for each emmision source type by the CEB method. R&D Vol. 29 No. 2 ( )

10 Table 5(b)F1 Cae Cao Cl K NO 3 NH 4 F2 Fe Pb MgCa F3 V Zn F4 Al Na b 12 q j f i j 0.05µg m 3 F1RUN 1 RUN 2 F2 F4 RUN 2 F3 RUN 2 RUN 3 Okamoto Pb C Sb Zn Br As 3 F3 F1 CEB F2 CEB RUN 1 2 RUN 4 F27 8 F2 F3 V CEB F3 SO F1 F3SO 4 (a) Factor loading and eigenvalues. (b) Varimax rotated factor loading. F1 F2 F3 F4 F1 F2 F3 F4 Cae Cao Na Mg Al K Ca V Fe Zn Pb NH Cl NO 3 2 SO Eigenvalues Cae Cao Na Mg Al K Ca V Fe Zn Pb NH Cl NO 3 2 SO : f 0.7, : 0.7 > f 0.6, f = factor loading R&D Vol. 29 No. 2 ( )

11 16 CEB F2 F4 CEB CEB 4 SPM 17 CEB (1) SPM 30700m 700m 2.5 (2) Fe V SPM (3) 6 7 Cae Na Al K Fe V Zn CEB (4) 154 F1 F2 Average contributions for each emission source type by factor analysis (FA) and CEB method. Change of "iron" contribution calculated (a) by CEB method, and (b) by factor analysis. (unit: µg/m 3 ) Source CEB Factor FA Diesel 17.4 Refuse F Secondary 12.6 Iron 2.1 F2 3.9 Heavy oil 1.3 F3 8.6 Soil 6.5 Sea salt F Unknown R&D Vol. 29 No. 2 ( )

2 F3SO 4 F4 (5) CEB 1) FriedlanderS. K. : "Chemical Element Balances and Identification of Air Pollution Sources"Environ. Sci. Tech.

: "The Effect Variance Weighting for Least Squares Calculations Applied to the Mass Balance Receptor Model"Atmos. Environ.-7(1984)1347 4) HopkeP. K., et al.

: "Identification of Aerosol Sources in the St. Louis Area Using Factor Analysis"J. Appl. Meteorol. (1978)600 6) LioyP. J., et al.

-11(1989)239 7) (1992)228 8) (1990)11 9) : " "26 (1985)133 10) 2 : " " (1979)296 11) 2 : " " (1979)190 12) 2 : " " (1979)69 13) : " "25(1984)600 14) 6 : "

: "The Relationship between the Chemical Mass Balance (CMB) and Absolute Principal Component Score (APCS) Receptor Model"84th Annual Meeting & Exhibition,

12 2 F3SO 4 F4 (5) CEB 1) FriedlanderS. K. : "Chemical Element Balances and Identification of Air Pollution Sources"Environ. Sci. Tech. -3(1973)235 2) " (I)" - 5(1980)198 3) WatsonJ. G., et al. : "The Effect Variance Weighting for Least Squares Calculations Applied to the Mass Balance Receptor Model"Atmos. Environ.-7(1984)1347 4) HopkeP. K., et al. : "The Use of Multivariate Analysis to Identify Sources of Selected Elements in the Boston Urban Aerosol"ibid(1976)1015 5) GatzD. F. : "Identification of Aerosol Sources in the St. Louis Area Using Factor Analysis"J. Appl. Meteorol. (1978)600 6) LioyP. J., et al. : "The Effect of Sampling Duration on the Ability to Resolve Source Types Using Factor Analysis" Atmos. Environ.-11(1989)239 7) (1992)228 8) (1990)11 9) : " "26 (1985)133 10) 2 : " " (1979)296 11) 2 : " " (1979)190 12) 2 : " " (1979)69 13) : " "25(1984)600 14) 6 : " " (1984)59 15) : " CMB "28(1987)146 16) : (1972)334 17) ThurstonG. D. and ItoK. : "The Relationship between the Chemical Mass Balance (CMB) and Absolute Principal Component Score (APCS) Receptor Model"84th Annual Meeting & Exhibition, VancouberBritish Columbia, (1991) Paper ) Na KarasawaM. and Kogiso T. : "Characterization of SPM Samples Collected before and after Typhoon Passage"Proc. Int. Symp. of Univ. of Osaka Prefect. on Global Amenity (1992)172 19) OkamotoS., et al. : "A Factor Analysis -Multiple Regression Model for Source Appotionment of Suspended Particulate Matter"Atmos. Enviorn. -8(1990) R&D Vol. 29 No. 2 ( )

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untitled 2 3 WHO (kd ) Lol p 1 grass group? 27 35 Lol p 2? 11 Lol p 3? 11 Lol p 4? 57 Lol p 5? 25 30 Lol p 9? 31 35 Lol p10 12 Lol p11 16 15 How about recent studies? Animal exposure Biomedical tests Questionnaire