Abstract
Sequential extraction integrated with isotope analysis was carried out on a sediment core from Liaodong Bay, northeast China, for characterizing Pb in various extraction phases and its possible sources. Results show that in all extracted fractions Pb concentrations increased abruptly in the top part of the sediments that deposited after 1980, but remained lower and rather constant before 1980. Consistent with the variation pattern of Pb concentration, the 206Pb/207Pb ratio displays a dramatic decrease around 1980. These findings strongly suggest serious Pb pollution since then. The Pb concentration and the isotopic ratios of 206Pb/207Pb and 208Pb/207Pb in the residual fraction show rather small changes through the entire core, and are similar to those of uncontaminated Chinese loess, possibly representing the characteristics of the regional geogenic background. The isotopic ratios of the sediments before 1980 varied in different extracted fractions with a linear pattern, from the residual at the highest toward the average signature of automobile exhausts and Pb-Zn deposits, implying a prominent two-end member mixing style of the Pb origin; one is the regional geologic background and the other is anthropogenic sources. The difference in isotopic ratios between the extractions might be indicative of varied proportions of the two sources. For sediments after 1980, however, the isotope ratios in nonresidual fractions are all relatively low and show little differentiation, which may suggest that polluted Pb dominates all the extracted fractions for the top part of the core.
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Adams WJ, Kimerle RA, Barnett JW Jr (1992) Sediment quality and aquatic life assessment. Environ Sci Technol 26:1865–1875
Alfonso S, Grousset F, MasseH L, Tastet JP (2001) A European lead isotope signal recorded from 6000 to 300 years BP in coastal marshes (SW France). Atmos Environ 35:3595–3605. doi:10.1016/S1352-2310(00)00566-5
Al-Masri MS, Al-Bich F (2002) Distribution of polonium-210 in Syrian phosphogypsum. J Radioanal Nucl Chem 251:3–9. doi:10.1023/A:1014834209326
Al-Masri MS, Al-Kharfan K, Al-Shamali K (2006) Speciation of Pb, Cu and Zn determined by sequential extraction for identification of air pollution sources in Syria. Atmos Environ 40:753–761. doi:10.1016/j.atmosenv.2005.10.008
Appleby PG (2001) Chronostratigraphic techniques in recent sediments. In: Last WM, Smol JP (eds) Tracking environmental change using lake sediments. Vol. 1: Basin analysis, coring and chronological techniques. Kluwer Academic, Dordrecht, pp 171–203
Appleby PG, Oldfield F (1978) The calculation of 210Pb dates assuming a constant rate of supply of unsupported 210Pb to the sediment. Catena 5:1–8. doi:10.1016/S0341-8162(78)80002-2
Appleby PG, Nolan PJ, Gifford DW, Godfrey MJ, Oldfield F, Anderson NJ, Battarbee RW (1986) 210Pb dating by low background gamma counting. Hydrobiologia 141:21–27. doi:10.1007/BF00026640
Audry S, Schäfer J, Blanc G, Jouanneau J (2004) Fifty-year sedimentary record of heavy metal pollution (Cd, Zn, Cu, Pb) in the Lot River reservoirs (France). Environ Pollut 132:413–426. doi:10.1016/j.envpol.2004.05.025
Bacon JR, Farmer JG, Dunn SM, Graham MC, Vinogradoff SI (2006) Sequential extraction combined with isotope analysis as a tool for the investigation of lead mobilisation in soils: application to organic-rich soils in an upland catchment in Scotland. Environ Pollut 141:469–481. doi:10.1016/j.envpol.2005.08.067
Biscaye PE, Grousset FE, Revel M, Vander G, Zielinski GA, Vaars A, Kukla G (1997) Asian provenance of glacial dust (stage 2) in the Greenland Ice Sheet Project 2 Ice Core, Summit, Greenland. J Geophys Res 102:26765–26781. doi:10.1029/97JC01249
Bollhöfer A, Mangini A, Lenhard A, Wessels M, Giovanioli F, Schwarz B (1994) High resolution 210Pb dating of Lake Constance sediments: stable lead in Lake Constance. Environ Geol 24:267–274. doi:10.1007/BF00767087
Borovec Z, Tolar V, Mraz L (1993) Distribution of some metals in sediments of the central part of the Labe (Elbe) River, Czech Republic. Ambio 22:200–205
Bruder-Hubscher V, Lagarde F, Leroy MJF, Coughanowr C, Enguehard F (2002) Application of a sequential extraction procedure to study the release of elements from municipal solid waste incineration bottom ash. Anal Chim Acta 451:285–295. doi:10.1016/S0003-2670(01)01403-9
Campanella L, Dorazio D, Petronio BM, Pietrantonio E (1995) Proposal for a metal speciation study in sediments. Anal Chim Acta 309:387–393. doi:10.1016/0003-2670(95)00025-U
Cunong DT, Obbard JP (2006) Metal speciation in coastal marine sediments from Singapore using a modified BCR-sequential extraction procedure. Appl Geochem 21:1335–1346. doi:10.1016/j.apgeochem.2006.05.001
Foster IDL, Boardman J, Keay-Bright J, Meadows ME (2005) Land degradation and sediment dynamics in the South African Karoo. Int Assoc Hydrol Sci Publ 292:207–213
Goldberg ED (1963) Geochronology with 210Pb. In radioactive dating. International Atomic Energy Agency, Vienna, pp 121–131
Gomezariza JL, Giraldez I, Sanchez-Rodas D, Moralesm E (2000) Metal sequential extraction procedure optimized for heavily polluted and iron oxide rich sediments. Anal Chim Acta 414:151–164. doi:10.1016/S0003-2670(00)00804-7
Hamilton TF, Ballestra S, Baxter MS, Gastaud J, Osvath I, Parsi P, Povinec PP, Scott EM (1994) Radiometric investigations of Kara Sea sediments and preliminary radiological assessment related to dumping of radioactive wastes in the Arctic Seas. J Environ Radioact 25:113–134. doi:10.1016/0265-931X(94)90011-6
Hinrichs J, Dellwig O, Brumsack HJ (2002) Lead in sediments and suspended particulate matter of the German bight: natural versus anthropogenic origin. Appl Geochem 17:621–632. doi:10.1016/S0883-2927(01)00124-X
Hlavay J, Prohaska T, Weisz M, Wenzel WW, Stingeder GJ (2004) Determination of trace elements bound to soils and sediments fractions. Pure Appl Chem 72:415–442. doi:10.1351/pac200476020415
Jha SK, Chavan SB, Pandit GG, Sadasivan S (2003) Geochronology of Pb and Hg pollution in a coastal marine environment using global fallout. J Environ Radioact 69:145–157. doi:10.1016/S0265-931X(03)00092-4
Jones B, Turki A (1997) Distributioin and speciation of heavy metals in surfical sediments from Tees Estuary, north-east England. Mar Pollut Bull 34:768–779. doi:10.1016/S0025-326X(97)00047-7
Kersten M, Förstner U (1986) Chemical fractionation of heavy metals in anoxic estuarine and coastal sediments. Water Sci Technol 18:121–130
Kersten M, Garbe-Schonberg C, Thomsen S (1997) Source apportionment of Pb pollution in the coastal water of Elefsis Bay, Greece. Environ Sci Technol 31:1295–1301. doi:10.1021/es960473z
Kober B, Wessels M, Bollhöfer A, Mangini A (1999) Pb isotopes in sediments of Lake Constance, Central Europe constrain the heavy metal pathways and the pollution history of the catchment, the lake and the regional atmosphere. Geochim Cosmochim Acta 63:1293–1303. doi:10.1016/S0016-7037(99)00064-2
Komárek M, Ettler V, Chrastný V, Mihaljevič M (2007) Lead isotopes in environmental sciences: a review. Environ Int. doi:10.1016/j.envint.2007.10.005
Lair GJ, Zehetner MGF, Gerzabek MH (2008) Distribution of cadmium among geochemical fractions in floodplain soils of progressing development. Environ Pollut 56: 207–214
Land M, Öhlander B, Ingri J, Thunberg J (1999) Solid speciation and fractionation of rare earth elements in a spodosol profile from northern Sweden as revealed by sequential extraction. Chem Geol 160:121–138. doi:10.1016/S0009-2541(99)00064-9
Li XD, Shen ZG, Wai WH, Li YS (2001) Chemical forms of Pb, Zn and Cu in the sediment profiles of the Pearl River estuary. Mar Pollut Bull 42:215–223. doi:10.1016/S0025-326X(00)00145-4
Mao D, Zhong C, Chen Z, Hu X (2001) Pb isotope characteristics of Pb-Zn-(Ag) deposits in the middle north margin of north China block:constraints on source process. Prog Precambr Res 24:193–198 (in Chinese)
Monna F, Ben Othman D, Luck JM (1995) Lead isotopes and Pb, Zn and Cd concentrations in the rivers feeding a coastal pond (Thau, southern France): constraints on the origin(s) and flux(es) of metals. Sci Total Environ 166:19–34. doi:10.1016/0048-9697(95)04514-2
Monna F, Loizeau JL, Thomas BA, Guéguen C, Favarger PY (1998) Pb and Sr isotope measurements by inductively coupled plasma-mass spectrometer: efficient time management for precision improvement. Spectrochim Acta Part B 53:1317–1333. doi:10.1016/S0584-8547(98)00164-5
Monna F, Dominik J, Loizeau JL, Pardos M, Arpagus P (1999) Origin and evolution of Pb in sediments of Lake Geneva (Switzerland-France). Establishing a stable Pb record. Environ Sci Technol 33:2850–2857. doi:10.1021/es9902468
Monna F, Clauer N, Toulkeridis T, Lancelot JR (2000) Influence of anthropogenic activity on the lead isotope signature of Thau Lake sediments (southern France):origin and temporal evolution. Appl Geochem 15:1291–1305. doi:10.1016/S0883-2927(99)00117-1
Mucha AP, Vasconcelos MTSD, Bordalo AA (2003) Macrobenthic community in the douro estuary: relations with trace metals and natural sediment characteristics. Environ Pollut 121:169–180. doi:10.1016/S0269-7491(02)00229-4
Mukai H, Furuta N, Fujii T, Ambe Y (1993) Characterisation of sources of lead in the urban air of Asia using ratios of stable isotopes. Environ Sci Technol 27:134756. doi: 10.1021/es00044a009
Mukai H, Tanaka A, Fujii T, Zeng Y, Hong Y, Sun Z, Zhou J, Xue D, Zhao J, Zhai G, Gu J, Zhai P (2001) Regional characteristics of sulfur and lead isotope ratios in the atmosphere at several Chinese urban sites. Environ Sci Technol 35:1064–1071. doi:10.1021/es001399u
Nakano T, Morohashi S, Yasuda H, Sakai M, Aizawa S, Shichi K, Morisawa T, Takahashi M, Sanada M, Matsuura Y, Sakai H, Akama A, Okada N (2006) Determination of seasonal and regional variation in the provenance of dissolved cations in rain in Japan based on Sr and Pb isotopes. Atmos Environ 40:7409–7420. doi:10.1016/j.atmosenv.2006.06.049
Rath P, Panda UC, Bhatta D, Sahu KC (2008) Use of sequential leaching, mineralogy, morphology and multivariate statistical technique for quantifying metal pollution in highly polluted aquatic sediments—A case study: Brahmani and Nandira Rivers, India. J Hazard Mater doi:10.1016/j.jhazmat.2008.07.048
Rauret G, Rubio R, Lopez-Sanchez JF (1989) Optimization of Tessier procedure for metal solid speciation in river sediments. Int J Environ Anal Chem 36:69–83. doi:10.1080/03067318908026859
Romas H, Gonzalez MJ, Hernandez LM (1999) Sequential extraction of copper, lead, cadmium, and zinic in sediments from Ebro river (Spain): relationship with level detected in earthworms. Bull Environ Contam Toxicol 62:301–308. doi:10.1007/s001289900874
Ruiz-Fernández AC, Hillaire-Marcel C, Páez-Osuna F, Ghaleb B, Soto-Jiménez M (2003) Historical trends of metal pollution recorded in the sediments of the Culiacan River Estuary, Northwestern Mexico. Appl Geochem 18:577–588. doi:10.1016/S0883-2927(02)00117-8
Sánchez-Martín MJ, García-Delgado M, Lorenzo LF, Rodríguez-Cruz MS, Arienzo M (2007) Heavy metals in sewage sludge amended soils determined by sequential extractions as a function of incubation time of soils. Geoderma 142:262–273. doi:10.1016/j.geoderma.2007.08.012
Segura R, Arancibia V, Zúñiga MC, Pastén P (2006) Distribution of copper, zinc, lead and cadmium concentrations in stream sediments from the Mapocho River in Santiago, Chile. J Geochem Explor 91:71–80. doi:10.1016/j.gexplo.2006.03.003
Shiharata H, Elias W, Patterson CC (1980) Chronological variations in concentrations and isotopic compositions of anthropogenic atmospheric lead in sediments of a remote subalpine pond. Geochim Cosmochim Acta 44:149–162. doi:10.1016/0016-7037(80)90127-1
Tessier A, Campbell PGC, Bisson M (1979) Sequential extraction procedure for the speciation of particulate trace metals. Anal Chem 51:844–851. doi:10.1021/ac50043a017
Torri SI, Lavado RS (2007) Dynamics of Cd, Cu and Pb added to soil through different kinds of sewage sludge. Waste Manage 28:821–832. doi:10.1016/j.wasman.2007.01.020
Yang Z, Lu W, Xin X, Li J, Li P (2008) Lead isotope signatures and source identification in urban soil of Changchun city. J Jilin Univ (Earth Sci Ed) 38:663–669
Zdenek B (1996) Evaluation of the concentrations of trace elements in stream sediments by factor and cluster analysis and the sequential extraction procedure. Sci Total Environ 177:237–250. doi:10.1016/0048-9697(95)04901-0
Zhang XL (2001) Investigation of pollution of Hg, Cd, Hg, As in sea water and deposit of Bohai Sea area. Environ J Heilongjiang 25:87–90
Zheng J, Tan M, Shibata Y, Tanaka A, Li Y, Zhang G, Zhang Y, Shan Z (2004) Characteristics of lead isotope ratios and elemental concentrations in PM10 fraction of airborne particulate matter in Shanghai after the phase-out of leaded gasoline. Atmos Environ 38:1191–1200. doi:10.1016/j.atmosenv.2003.11.004
Acknowledgments
The authors thank Professor Zhaohui Wu for help with elemental and isotopic analysis. The critical review and constructive comments of Editor D. R. Doerge and two anonymous reviewers are greatly appreciated; they led to substantial improvement of the paper. This work was funded by the National Natural Science Foundation (40672118).
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Xu, B., Gu, Z., Han, J. et al. Sequential Extractions and Isotope Analysis for Discriminating the Chemical Forms and Origins of Pb in Sediment from Liaodong Bay, China. Arch Environ Contam Toxicol 57, 230–238 (2009). https://doi.org/10.1007/s00244-008-9268-5
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DOI: https://doi.org/10.1007/s00244-008-9268-5