Gao, H.

Ghim, Y.

Grados, A.

Huehnerfuss, H.

Lammel, G.

Lohmann, R.

English

MPG.PuRe

C:\web sites\PDF_Test\pdf\817.pdfIntroduction Eastern China‘s economy is developing extremely rapid which has created significant pressure to the environment, even on a regional scale. 1-3 Despite the suspected significance of China as a source area, there are only extremely scarce data on organochlorine compounds are available from the atmospheric environment. Polychlorinated biphenyls (PCBs) have been observed in the air of cities of South China and concentrations in the range 350-700 pg m-3 were found. 2 Obviously, much more PCBs had been released into the environment in China than anticipated based on usage data. 4,5 The purpose of this study was to investigate the levels of organochlorines in eastern China and to address the regional transport of these pollutants in the Yellow and East China Seas region through simultaneous sampling at a coastal and an island site. Materials and Methods The measurements were performed 6-22 June 2003 at a coastal site, Qingdao, eastern China, and an island site, Gosan, on Jeju (Fig. 1, Table 1). The distance between the sites is about 500 km. The large-scale weather situation was characterized by a cyclone which moved from NW China (Heilongjiang) to the Yellow Sea and stayed there, and anti-cyclones over the TaklaMakan desert / Tibetan plateau, moving N to the Gobi desert, and over the South China Sea. During the entire campaign Qingdao was influenced by the cyclone while Jeju was under its influence from 11-17 June, until a typhoon approached from the S. Advection above the boundary layer (in 700 hPa) at the sites was from W-SW over Qingdao during the entire campaign and over Jeju first from S-SW (9-12 June), then from W (13-17 June) and finally again from S (17-21 June). Samples from Qingdao were analysed for hexachlorobenzene (HCB), hexachlorocyclohexanes (a-, b-, g-, d-, e-isomers), polychlorinated biphenyls (PCB congeners #28, 52, 101, 153, 180), 1,1,1-trichloro-2,2-bis-chlorophenylethanes and derivatives (DDTs, i.e. o,p’- and p,p’-DDD, -DDE and -DDT), drins (aldrin, dieldrin, endrin). Samples from Gosan were analysed for HCHs (a-, b-, g-isomers) and PCB (congeners #28, 52, 77, 81, 101, 114, 118, 123, 126, 138, 153, 156, 167, 169, 170, 180, 189) using similar methods (Table 1). ORGANOCHLORINE COMPOUNDS IN AIR AT THE YELLOW SEA - MEASUREMENTS IN QINGDAO, CHINA, AND GOSAN, JEJU ISLAND, KOREAGerhard Lammel1, Young-Sung Ghim2, Amélie Grados1, Heinrich Hühnerfuss3, Rainer Lohmann1, Huiwang Gao4 1Max Planck Institute For Meteorology 2Air Resources Research Center, Korea Institute of Science and Technology 3Organomarine Chemistry, University of Hamburg 4Institute for the Marine Environment, Ocean University of ChinaEMV - Sources of POPs in the Pacific Rim496Fig. 1: Map of coastal and island sites, Qingdao and Gosan Table 1: Sampling and analysis characteristics at Qingdao and Gosan Results and Discussion The concentrations retained by filter membranes as well as by polyurethane foams (PUFs) placed downstream were below detection limits in many cases. The particulate fraction of organochlorines, according to the amount found in Site Qingdao, China Gosan, KoreaLocation 36°05'N, 120°20'E 78 m asl, 500 from coast33°17'N, 126°10'E 70 m asl, on cliff, western shoreSite type urban (7 million inhabitants in the wider area)rural (0.5 mn inhabitants on the island)Sampling period 9-21 June 2003,  6 day-time samples lacking 6-22 June 2003 2 24-h samples lacking Number of samples9 (4 day-time, 5 night-time) 15 (HCHs), 5 (PCBs)Sampling time 1-4 11-hour intervals combined1 (HCHs) or 3 (PCBs) 23-hour intervals combinedGas sampling PUF (5 cm high, 2-4 in series), 26 ± 3 m3 h-1 PUF (5 cm high), 60 m3 h-1 Particulate matter samplingquartz filter (Munktell, 79 cm2), no upper size cut-off, 26 ± 3 m3 h-1 Teflon filter (Gelman Zefluor) cut size 10 mm, 1.0 m3 h-1 Sample preparationExtraction (acetone), fractions separation (silica-alumina column)Analysis GC-EPD (column DB5) GC-EPD Determination limit (d.l.)0.2-5 ng per PUF sample and 0.2-10 ng per filter membrane corresponding to 1-120 (typically 10-20) pg m-3 per sampling train for individual substancescorresponding to 0.01-0.1 pg m-3 per sampling train for individual substancesEMV - Sources of POPs in the Pacific Rim497the filter vs. found in the PUFs, was negligible in most cases with some exceptions for drins and DDTs.  Many organochlorines including persistent organic pollutants (POPs) were found at significant to high concentration levels in air at the coastal urban site (Table 2). At the same time some other air pollutants, e.g. heavy metals, were elevated, too. 6 Air pollution was highest in samples collected at least partly during advection from W and N. This points to local sources within the urban area: Many industries are located along the Jiaozhou Bay shore (cf. Fig. 1). By average, night-time concentrations exceeded day-time concentrations (µnight/µday > 1) for most of the trace substances, while no significant deviation from 1 was found for the heavier PCBs (one penta- and one hexa-chloro congener; Table 2). µnight/µday > 1 points to local sources at the ground, while µnight/µday £  1 may indicate advection of pollutants (regional-scale pollution or long-range atmospheric transport) or local emissions which are stronger during day-time.  In general lower concentration levels of HCHs and PCBs were found at the island site confirming the background character. 7 The concentration gradient between the sites was > 5 for a -HCH and endrin and > 30 for the PCBs, i.e. similar to the concentration gradients found for heavy metals measured in parallel. 6 However, the gradient is smaller ( £  3) for b-HCH, g-HCH, DDTs and aldrin. In combination with the findings of night vs. day levels (above) it can be concluded that regional distribution or long-range atmospheric transport, possibly in combination with secondary sources (re-emission) are indicated for b-HCH, g-HCH, DDTs and aldrin. This would be in line with the perception of the fate of persistent substances. Rather high DDT/total-DDTs ratios point to recent DDT usage, though. DDT was banned in China in 1983. In contrast, the east China coastal region seems to be an active source region of a-HCH, endrin and, in particular, PCBs. The heavier ones may be subject to significantly stronger emissions during day-time, which could be caused by the diurnal temperature variation. With respect to PCBs and DDTs, the observed atmospheric concentrations are comparable with earlier results reported for cities of south China a few years ago. 2 Rather high values of a -/g -HCH are surprising as technical HCH, the source of a -HCH in the environment, was phase out in China in the 1980s We are not aware of any measurements of HCHs in China to compare our findings with. Table 2: Organochlorines’ and selected elemental concentrations and concentration ratios (day/night). Data are given in the form time-weightedmean (µ), minimum and maximum (min-max) in pg m-3 (ng m-3 for Ca, Pb) For values < d.l. half of the d.l. was used for the calculation of the mean value. Qingdao GosanSpecies µ min-max µnight/µday µ min-maxHCB 123 73-217 1.4a-HCH 145 10-277 2.2 20 6-34 b-HCH 72 < 3-400 96 21-223 g-HCH 68 < 13-132 2.0 21 6-60 d-HCH 19 < 2-62 e-HCH 109 < 36-345 PCB-28 113 < 10-248 4.5 1.7 0.6-3.7 PCB-52 25 < 7-59 0.9 0.4-1.4 PCB-101 27 < 6-81 0.28 0.15-0.37 PCB-153 47 < 6-207 0.9 0.16 0.09-0.21 PCB-180 98 < 6-448 0.7 0.06 0.02-0.12o,p’-DDT 45 < 1-101 1.5o,p’-DDE 16 < 1-32 1.9p,p’-DDE 32 < 2-72 0.7o,p’-DDD 14 < 6-33p,p’-DDD 70 26-163 1.9Adrin 1.2 < 0.6-12Dieldrin < 5.4Endrin 33 < 5-366Total HCHs 414 < 168-1132 3.4 138 55-271EMV - Sources of POPs in the Pacific Rim498(a) one main species, p,p'-DDDT, not measured, (b) encompass different substances at the two sites Acknowledgement We are grateful to Lifang Sheng and Mingyan Qiu, Ocean University of China, for providing excellent logistics and supporting trace gas data at the Qingdao site. This research received partly support by the German Federal Ministry of Education and Research (BMBF) and the Korean Ministry of Environment (KME). References 1. APERC (2004), Energy in China, Asia Pacific Energy Research Centre, Tokyo. 2. UNEP-Chemicals (2002): Regionally based assessment of persistent toxic substances, Central and North east Asia regional report, 125 pp., available as  3. Zhang, Y.J., Gao, H.W. (2001) in: Slowly degradable organics in the atmospheric environment and air -sea exchange (Lammel G., ed.), Report Max Planck Institute for Meteorology No. 335, Hamburg, Germany, pp. 9-20 4. Jiang, K., Li, L.J., Chen, Y.D., Jin, J. (1997), Chemosphere 34: 941-950. 5. Zang, W.C., Chongyano, J. (2000) in: UNEP-Chemicals, Proceedings of the Subregional Workshop on Identification and Management of Dioxins/Furans and PCBs, Seoul 24.-28.7.2000, pp. 73-76,  6. Lammel G., Ghim Y.S., Broekaert J.A.C., Gao H.W. (2005), submitted 7. Arimoto R., Duce R.A., Savoie D.L., Prospero J.M., Talbot R., Cullen J.D., Tomza U., Lewis N.F., Ray, B.J. (1996) J. Geophys. Res. 101: 2011-2023. Total PCBs 310 66-567 1.6 3.7 1.6-6.8Total DDTs 176 (b) 86-285 1.5Total drins 37 < 11-369a -/g-HCH 2.1 1.7- > 8.5 - 1.2 0.5-2.7DDT/totalDDTs 0.44 < 0.03-0.86 1.7 0.35 0.22-0.51Ca 830 500–2410 1.4 87 37-122Pb 102 28-215 2.6 13 2-34EMV - Sources of POPs in the Pacific Rim499

Organochlorine compounds in air at the Yellow Sea: measurements in Qingdao, China, and Gosan, Jeju Island, Korea

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Organochlorine compounds in air at the Yellow Sea: measurements in Qingdao, China, and Gosan, Jeju Island, Korea

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