Historical occurrences of polybrominated diphenyl ethers and polychlorinated biphenyls in Manila Bay, Philippines, and in the upper Gulf of Thailand

Historical trends of the accumulation of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) in a typical tropical Asian environment were investigated using radio-dated sediment cores from Manila Bay, the Philippines and from the upper Gulf of Thailand. Vertical profiles indicated earlier usage of PCBs than of PBDEs which coincided with their industrial production. The increasing concentrations of total PBDEs and PCBs toward the surface suggested an increased consumption of PBDEs; and possible leakage of PCBs from old machineries into the aquatic environment in recent years. Current input of PCBs to the catchment of Manila Bay was supported by the analyses of air samples and plastic resin pellets. The vertical profiles of total PBDEs in the cores (i.e., rapidly increasing concentrations corresponding to the mid-1980s until mid-1990s, followed by a decrease until the early 2000s, and increasing again toward the surface) likely corresponded to the rapid economic growth in Asia in the 1990s, the Asian financial crisis in 1997, and the economic recovery since early 2000s. BDE-209 was predominant especially on the surface layers. BDEs 47 and 99 generally decreased toward the surface, reflecting the phase-out of the technical penta-PBDE products and the regulation by the Stockholm Convention in recent years. Increasing ratios of BDE-202/209, 206/209, 207/209 and decreasing % of BDE-209 down the core layers may provide evidence for the anaerobic debromination of BDE-209 in the sediment cores. Inventories in ng/cm2 of total PCBs were higher than total PBDEs (92 vs. 34 and 47 vs. 11 in the Philippines; 47 vs. 33 in Thailand). However, the doubling times indicated faster accumulation of total PBDEs (6–7 years) and BDE-209 (6–7.5 years) than of PCBs (8–11 years). Furthermore, the temporal increase in BDE-209 was comparable to or faster than those reported in other water bodies around the world

Sources of sedimentary PAHs in tropical Asian waters: differentiation between pyrogenic and petrogenic sources by alkyl homolog abundance

We collected surface sediment samples from 174 locations in India, Indonesia, Malaysia, Thailand, Vietnam, Cambodia, Laos, and the Philippines and analyzed them for polycyclic aromatic hydrocarbons (PAHs) and hopanes. PAHs were widely distributed in the sediments, with comparatively higher concentrations in urban areas (∑PAHs: ∼1000 to ∼100 000 ng/g-dry) than in rural areas (∼10 to ∼100 g-dry), indicating large sources of PAHs in urban areas. To distinguish petrogenic and pyrogenic sources of PAHs, we calculated the ratios of alkyl PAHs to parent PAHs: methylphenanthrenes to phenanthrene (MP/P), methylpyrenes + methylfluoranthenes to pyrene + fluoranthene (MPy/Py), and methylchrysenes + methylbenz[a]anthracenes to chrysene + benz[a]anthracene (MC/C). Analysis of source materials (crude oil, automobile exhaust, and coal and wood combustion products) gave thresholds of MP/P = 0.4, MPy/Py = 0.5, and MC/C = 1.0 for exclusive combustion origin. All the combustion product samples had the ratios of alkyl PAHs to parent PAHs below these threshold values. Contributions of petrogenic and pyrogenic sources to the sedimentary PAHs were uneven among the homologs: the phenanthrene series had a greater petrogenic contribution, whereas the chrysene series had a greater pyrogenic contribution. All the Indian sediments showed a strong pyrogenic signature with MP/P ≈ 0.5, MPy/Py ≈ 0.1, and MC/C ≈ 0.2, together with depletion of hopanes indicating intensive inputs of combustion products of coal and/or wood, probably due to the heavy dependence on these fuels as sources of energy. In contrast, sedimentary PAHs from all other tropical Asian cities were abundant in alkylated PAHs with MP/P ≈ 1–4, MPy/Py ≈ 0.3–1, and MC/C ≈ 0.2–1.0, suggesting a ubiquitous input of petrogenic PAHs. Petrogenic contributions to PAH homologs varied among the countries: largest in Malaysia whereas inferior in Laos. The higher abundance of alkylated PAHs together with constant hopane profiles suggests widespread inputs of automobile-derived petrogenic PAHs to Asian waters

International Pellet Watch: global monitoring of persistent organic pollutants (POPs) in coastal waters. 1. Initial phase data on PCBs, DDTs, and HCHs

Samples of polyethylene pellets were collected at 30 beaches from 17 countries and analyzed for organochlorine compounds. PCB concentrations in the pellets were highest on US coasts, followed by western Europe and Japan, and were lower in tropical Asia, southern Africa and Australia. This spatial pattern reflected regional differences in the usage of PCBs and was positively correlated with data from Mussel Watch, another monitoring approach. DDTs showed high concentrations on the US west coast and in Vietnam. In Vietnam, DDT was predominant over its metabolites (DDE and DDD), suggesting the principal source may be current usage of the pesticide for malaria control. High concentrations of pesticide HCHs were detected in the pellets from southern Africa, suggesting current usage of the pesticides in southern Africa. This study demonstrates the utility and feasibility of the International Pellet Watch approach to monitor POPs at a global scale

International pellet watch: global monitoring of persistent organic pollutants(POPs) in coastal waters. 1. Initial phase data on PCBs, DDTs, and HCHs

Samples of polyethylene pellets were collected at 30 beaches from 17 countries and analyzed for organochlorine compounds. PCB concentrations in the pellets were highest on US coasts, followed by western Europe and Japan, and were lower in tropical Asia, southern Africa and Australia. This spatial pattern reflected regional differences in the usage of PCBs and was positively correlated with data from Mussel Watch, another monitoring approach. DDTs showed high concentrations on the US west coast and in Vietnam. In Vietnam, DDT was predominant over its metabolites (DDE and DDD), suggesting the principal source may be current usage of the pesticide for malaria control. High concentrations of pesticide HCHs were detected in the pellets from southern Africa, suggesting current usage of the pesticides in southern Africa. This study demonstrates the utility and feasibility of the International Pellet Watch approach to monitor POPs at a global scale

Facilitated Leaching of Additive-Derived PBDEs from Plastic by Seabirds’ Stomach Oil and Accumulation in Tissues

Our previous study suggested the transfer of polybrominated diphenyl ether (PBDE) flame retardants from ingested plastics to seabirds’ tissues. To understand how the PBDEs are transferred, we studied leaching from plastics into digestive fluids. We hypothesized that stomach oil, which is present in the digestive tract of birds in the order Procellariiformes, acts as an organic solvent, facilitating the leaching of hydrophobic chemicals. Pieces of plastic compounded with deca-BDE were soaked in several leaching solutions. Trace amounts were leached into distilled water, seawater, and acidic pepsin solution. In contrast, over 20 times as much material was leached into stomach oil, and over 50 times as much into fish oil (a major component of stomach oil). Analysis of abdominal adipose, liver tissue, and ingested plastics from 18 wild seabirds collected from the North Pacific Ocean showed the occurrence of deca-BDE or hexa-BDEs in both the tissues and the ingested plastics in three of the birds, suggesting transfer from the plastic to the tissues. In birds with BDE209 in their tissues, the dominance of BDE207 over other nona-BDE isomers suggested biological debromination at the meta position. Model calculation of PBDE exposure to birds based on the results of the leaching experiments combined with field observations suggested the dominance of plastic-mediated internal exposure to BDE209 over exposure via prey

Monitoring of a wide range of organic micropollutants on the Portuguese coast using plastic resin pellets

We analyzed polychlorinated biphenyls (PCBs), dichlorodiphenyl dichloroethane and its metabolites, hexachlorocyclohexanes (HCHs), polycyclic aromatic hydrocarbons (PAHs), and hopanes, in plastic resin pellets collected from nine locations along the Portuguese coast. Concentrations of a sum of 13 PCBs were one order of magnitude higher in two major cities (Porto: 307. ng/g-pellet; Lisboa: 273. ng/g-pellet) than in the seven rural sites. Lower chlorinated congeners were more abundant in the rural sites than in the cities, suggesting atmospheric dispersion. At most of the locations, PAH concentrations (sum of 33 PAH species) were ∼100 to ∼300. ng/g-pellet; however, three orders of magnitude higher concentrations of PAHs, with a petrogenic signature, were detected at a small city (Sines). Hopanes were detected in the pellets at all locations. This study demonstrated that multiple sample locations, including locations in both urban and remote areas, are necessary for country-scale pellet watch.This research was financially supported by Mitsui and Co. Ltd., Environment Fund for their financial support (Project R11-G4-1053) and Grants-in-Aid from the Ministry of Education and Culture of Japan (Project No. 22254001). We also appreciate to be supported by Fundação para a Ciência e Tecnologia, Portugal for their financial support through the project POIZON reference PTDC/MAR/102677/2008 and fellowship reference SFRH/BD/74772/2010.publishe