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Residue of DDT and HCH in Fish from Lakes and Rivers in the World

Written By

Taizo Tsuda

Submitted: 19 December 2011 Published: 01 August 2012

DOI: 10.5772/48725

From the Edited Volume

Pesticides - Recent Trends in Pesticide Residue Assay

Edited by R.P. Soundararajan

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1. Introduction

Organochlorine pesticides such as DDT and HCH had been abundantly produced and used since the around twentieth century in all over the world and environmental pollution, food contamination and human body pollution had developed into social problem because of their high bioconcentration potential and high persistency. The use and manufacturing of DDT and HCH were forbidden in many countries including Japan in all over the world in the first half in 1970's.

In Japan, the use of organochlorine pesticides registered in persistent organic pollutants (POPs) was prohibited, for example, in 1971 for DDT and HCH and in 1986 for chlordane. Levels of DDT and HCH have been monitored annually in wildlife such as fish, shellfish and bird from a freshwater lake, 17 sea areas and 2 land areas in Japan since 1979 [1-31]. Lake Biwa, the largest in Japan, was selected as a freshwater lake and a freshwater fish, Japanese dace from the lake was selected as a wildlife sample.

In the world, a few reports have been published for long-term monitoring of POPs in aquatic biota from lakes only in USA and Sweden. In USA, the use of DDT was prohibited in 1972. Levels of POPs such as DDT, chlordanes, Mirex, Dieldrin have been monitored annually in fish from the Grate Lakes since 1970 [32, 33]. In Sweden, the use of DDT was prohibited in 1970. Levels of DDT, HCB and HCH have been monitored annually in fish from Lake Storvindeln since 1968 [34].

On the other hand, many field data have been published for temporal monitoring of DDT and HCH in fish from lakes [35-70] and rivers [40, 51, 68, 71-101].

This study was performed for the accumulation of fundamental data on DDT and HCH contamination of fish in lakes and rivers in the world to evaluate their concentration changes by POPs Regulation. The data were collected from the published reports in which the accuracy in the chemical analyses of the pesticides was over the standard level. This chapter consisted of (1) Residue of T-DDT and T-HCH in fish from lakes and rivers in the world, (2) Long-term trends of T-DDT and T-HCH in fish from lakes in the world, (3) Composition of T-DDT and T-HCH in fish from lakes and rivers in the world.

  1. Each of the T-DDT and T-HCH concentration data in fish from lakes and rivers was compared for the 38 lakes surveyed in 8 countries of Europe and America and 8 countries of Asia and Africa from 1995 to 2008 and for the 28 rivers surveyed in 8 countries of Europe and America, 4 countries of Asia, Africa and Oceania from 2000 to 2009.

  2. Long-term trends of T-DDT and T-HCH in Japanese dace from Lake Biwa were shown from 1979 to 2009 and half-lives (t1/2) were calculated for T-DDT and T-HCH. The t1/2 values were 9 years for T-DDT and 4 years for T-HCH. Similarly, long-term trends of T-DDT in fish from Lake Biwa, Lake Ontario, Lake Michigan and Lake Storvindeln were shown and the t1/2 values of T-DDT were calculated. The t1/2 values were 9, 11, 8 and 7 years, respectively, in Lake Biwa, Lake Ontario, Lake Michigan and Lake Storvindeln. There were no wide differences in the t1/2 values between the four lakes.

  3. Composition of T-DDT in fish from lakes and rivers in the world was compared for the 25 lakes in 15 countries of Europe, America, Asia and Africa from 1996 to 2008 and for the 16 rivers in 8 countries of Europe, America, Asia, Africa and Oceania from 2000 to 2009. Similarly, composition of T-HCH in fish from lakes and rivers in the world was compared for the 16 lakes in 8 countries of Europe, America, Asia and Africa from 1996 to 2008 and for the 11 rivers in 5 countries of Europe and Asia from 2001 to 2006.

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2. Residue of T-DDT and T-HCH in fish from lakes and rivers in the world

Residue of T-DDT and T-HCH in fish from lakes and rivers in the world (Survey years: 1995∼2009) was reviewed from literatures in the past. The residue data were summarized in Table 1 for the lakes [22-31, 35-70] and in Table 2 for the rivers [40, 51, 68, 71-101].

No.SpeciesnaAnalyteLakeYearCountryT-HCH bT-DDT cReferences
L-1Japanese dace5MuscleLake Biwa2000Japan3 ng/g wet wt13 ng/g wet wtMinistry of the Environment, Japan (2002)
L-2Japanese dace5MuscleLake Biwa2001Japan2 ng/g wet wt10 ng/g wet wtMinistry of the Environment, Japan (2003)
L-3Japanese dace5MuscleLake Biwa2002Japan1.79 ng/g wet wt6.5 ng/g wet wtMinistry of the Environment, Japan (2004)
L-4Japanese dace5MuscleLake Biwa2003Japan0.97 ng/g wet wt8.0 ng/g wet wtMinistry of the Environment, Japan (2005)
L-5Japanese dace5MuscleLake Biwa2004Japan0.55 ng/g wet wt8.4 ng/g wet wtMinistry of the Environment, Japan (2006)
L-6Japanese dace5MuscleLake Biwa2005Japan0.29 ng/g wet wt9.3 ng/g wet wtMinistry of the Environment, Japan (2007)
L-7Japanese dace5MuscleLake Biwa2006Japan0.90 ng/g wet wt8.3 ng/g wet wtMinistry of the Environment, Japan (2008)
L-8Raibow trout (male)4MuscleLake Mashu2003Japan2.98 ng/g wet wt1.49 ng/g wet wtTakazawa et al. (2005)
L-9Raibow trout (female)6MuscleLake Mashu2003Japan2.71 ng/g wet wt1.72 ng/g wet wtTakazawa et al. (2005)
L-10Japanese dace (male)3MuscleLake Mashu2003Japan1.75 ng/g wet wt0.66 ng/g wet wtTakazawa et al. (2005)
L-11Japanese dace (female)6MuscleLake Mashu2003Japan2.45 ng/g wet wt0.56 ng/g wet wtTakazawa et al. (2005)
L-12Raibow trout (male)3MuscleLake Mashu2002Japan3.23 ng/g wet wt3.50 ng/g wet wtTakazawa et al. (2005)
L-13Raibow trout (female)9MuscleLake Mashu2002Japan2.19 ng/g wet wt1.27 ng/g wet wtTakazawa et al. (2005)
L-14Unkown6WholeTaihu Lake Region1999∼2000China46 ng/g wet wt12 ng/g wet wtFeng et al. (2003)
L-15Carp3WholeLake Tai2000China64 ng/g fat wt980 ng/g fat wtNakata et al. (2005)
L-16Topmouth culter3WholeLake Tai2000China67 ng/g fat wt750 ng/g fat wtNakata et al. (2005)
L-17Spotted steed3WholeLake Tai2000China75 ng/g fat wt700 ng/g fat wtNakata et al. (2005)
L-18Catfish3WholeLake Tai2000China68 ng/g fat wt1000 ng/g fat wtNakata et al. (2005)
L-19Gymoncypris namensis4MuscleNam Co Lake2005China2.57 ng/g wet wt17.2 ng/g wet wtYang et al. (2007)
L-20Gymoncypris waddellii4MuscleYamdro Lake2005China1.56 ng/g wet wt2.76 ng/g wet wtYang et al. (2007)
L-21C. auratus8Edible partGaobeidian Lake (Beijing)2006China6.41 ng/g wet wt21.96 ng/g wet wtLi et al. (2008)
L-22M. anguillicaudatus5Edible partGaobeidian Lake (Beijing)2006China2.61 ng/g wet wt14.08 ng/g wet wtLi et al. (2008)
L-23H. leuciscultures8Edible partGaobeidian Lake (Beijing)2006China11.14 ng/g wet wt84.4 ng/g wet wtLi et al. (2008)
L-24Herbivorous9MuscleSongkhla Lake (Thale Luang)1997Thailand170 ng/g fat wtKumblad et al. (2001)
L-25Herbivorous10MuscleSongkhla Lake (Thale Sap)1997Thailand36 ng/g fat wtKumblad et al. (2001)
L-26Herbivorous8MuscleSongkhla Lake (Thale Sap Songkhla)1997Thailand35 ng/g fat wtKumblad et al. (2001)
L-27Channa striata64MuscleKolleru LakeUnkownIndiaAmaraneri & Pillala (2001)
L-28Channa striata56LiverKolleru LakeUnkownIndiaAmaraneri & Pillala (2001)
L-29Catla catla58MuscleKolleru LakeUnkownIndiaAmaraneri & Pillala (2001)
L-30Catla catla38LiverKolleru LakeUnkownIndiaAmaraneri & Pillala (2001)
L-31P. phuturio2WholeHaleji Lake1999Pakistan4.55 ng/g wet wtSanpera et al. (2002)
L-32C. lalia3WholeHaleji Lake1999Pakistan5.58 ng/g wet wtSanpera et al. (2002)
L-33G. giuris1WholeHaleji Lake1999Pakistan5.94 ng/g wet wtSanpera et al. (2002)
L-34Several kinds81Edible partLake Jarun2000Croatia0.40 ng/g wet wt*0.80 ng/g wet wt*Bosnir et al. (2007)
L-35Arctic char25MuscleLake Ellasjøen1996Norway60 ng/g wet wtEvenset et al. (2004)
L-36Arctic char12MuscleLake Øyangen1996Norway4.3 ng/g wet wtEvenset et al. (2004)
L-37Whitefish (Female) 100-200g13MuscleLake Stuorajavri2005NorwayND0.35 ng/g wet wtChristensen et al. (2007)
L-38Whitefish (Male) 100-200g10MuscleLake Stuorajavri2005NorwayND0.41 ng/g wet wtChristensen et al. (2007)
L-39Pike5MuscleLake Stuorajavri2005NorwayND0.24 ng/g wet wtChristensen et al. (2007)
L-40Brown trout1MuscleL. Tuma (remote alpine lake)2003Switzerland1100 ng/g fat wt (+op')Schmid et al. (2007)
L-41Brown trout1MuscleL. Moesola (remote alpine lake)2003Switzerland680 ng/g fat wt(+op')Schmid et al. (2007)
L-42Lake trout1MuscleL. Diavolezza (remote alpine lake)2003Switzerland130 ng/g fat wt(+op')Schmid et al. (2007)
L-43Catfish8MuscleLake Trasimeno1998Italy14.3 ng/g fat wt216 ng/g fat wtElia et al. (2006)
L-44Mullet (Lisa aurata)13MuscleLake Ganzirri2001Italy3.8 ng/g wet wt (Max.)Licata et al. (2003)
L-45Landlocked5WholeLake Maggiore2002-2004Italy2500 ng/g fat wtBettinetti et al. (2006)
L-46Whitefish5WholeLake Maggiore2002-2004Italy1370 ng/g fat wtBettinetti et al. (2006)
L-47Perch5WholeLake Maggiore2002-2004Italy1860 ng/g fat wtBettinetti et al. (2006)
L-48Chub5WholeLake Maggiore2002-2004Italy1190 ng/g fat wtBettinetti et al. (2006)
L-49Rudd5WholeLake Maggiore2002-2004Italy2770 ng/g fat wtBettinetti et al. (2006)
L-50Tench5WholeLake Maggiore2002-2004Italy2720 ng/g fat wtBettinetti et al. (2006)
L-51Perch1MuscleBolsena Lake2002Italy0.02 ng/g wet wt2.26 ng/g wet wtOrban et al. (2007)
L-52Perch1MuscleBracciano Lake2002Italy0.09 ng/g wet wt0.38 ng/g wet wtOrban et al. (2007)
L-53Perch1MuscleSalto Lake2002Italy0.03 ng/g wet wt0.61 ng/g wet wtOrban et al. (2007)
L-54Pelagic landlocked shad1MuscleLake Como (Como branch)2006Italy1010 ng/g fat wtBettinetti et al. (2008)
L-55Pelagic landlocked shad1MuscleLake Como (Como branch)2007Italy840 ng/g fat wtBettinetti et al. (2008)
L-56Pelagic landlocked shad1MuscleLake Como (Lecco branch)2007Italy610 ng/g fat wtBettinetti et al. (2008)
L-57Pelagic landlocked shad1MuscleLake Iseo2007Italy570 ng/g fat wtBettinetti et al. (2008)
L-58Pikeperch4MuscleBeysehir LakeUnkownTurkey70 ng/g wet wt27 ng/g wet wtAktumsek et al. (2002)
L-59Carp17MuscleSir Dam Lake2003Turkey0.21 ng/g wet wt*14.4 ng/g wet wt*Erdogrul et al. (2005)
L-60Oresochromus niloticus4MuscleLake Burullus2006Egypt1.88 ng/g wet wt5.13 ng/g wet wtSaid et al. (2008)
L-61Clarries sp.4MuscleLake Burullus2006Egypt9.83 ng/g wet wt12.54 ng/g wet wtSaid et al. (2008)
L-62Bagrus meridionalis4MuscleLake Malawi1996, 1997East Africa13.1 ng/g wet wtKidd et al. (2001)
L-63Buccochromis nototaenia2MuscleLake Malawi1996, 1997East Africa3.4 ng/g wet wtKidd et al. (2001)
L-64Clarius sp.1MuscleLake Malawi1996, 1997East Africa1.4 ng/g wet wtKidd et al. (2001)
L-65Engraulicyprus sardella6WholeLake Malawi1996, 1997East Africa4.5 ng/g wet wtKidd et al. (2001)
L-66Genyochromis mento5WholeLake Malawi1996, 1997East Africa1.0 ng/g wet wtKidd et al. (2001)
L-67Labeotropheus fuelleborni6WholeLake Malawi1996, 1997East Africa1.1 ng/g wet wtKidd et al. (2001)
L-68Boulengerochromis microlepis1WholeLake Tanganyika (North end)1999Burundi288.2 ng/g fat wt794.7 ng/g fat wtManirakiza et al. (2002)
L-69Chrysichthys sianenna1WholeLake Tanganyika (North end)1999Burundi90.6 ng/g fat wt339.3 ng/g fat wtManirakiza et al. (2002)
L-70Oreochromis niloticus1WholeLake Tanganyika (North end)1999Burundi66.2 ng/g fat wt393.1 ng/g fat wtManirakiza et al. (2002)
L-71Limnothrissa miodon1WholeLake Tanganyika (North end)1999Burundi21.2 ng/g fat wt60.7 ng/g fat wtManirakiza et al. (2002)
L-72Stolothrissa tanganyikae1WholeLake Tanganyika (North end)1999Burundi55.1 ng/g fat wt95.7 ng/g fat wtManirakiza et al. (2002)
L-73Nile tilapia43Edible partLake Victoria (Napoleon Gulf)1998Uganda1.39 ng/g wet wtKasozi et al. (2006)
L-74Nile perch37Edible partLake Victoria (Napoleon Gulf)1998Uganda1.67 ng/g wet wtKasozi et al. (2006)
L-75Nile tilapia and Nile perchMuscleLake Victoria (Kome Island)1999Tanzania20 ng/g wet wtHenry & Kishimba (2006)
L-76Nile tilapia and Nile perchMuscleLake Victoria (Katunguru)1999Tanzania15 ng/g wet wtHenry & Kishimba (2006)
L-77Nile tilapia10MuscleLake TaaboUnkownCote d'Ivoire225.8 ng/g dry wt124.1 ng/g dry wtRoche et al. (2007)
L-78African catfish7MuscleLake TaaboUnkownCote d'Ivoire130.0 ng/g dry wt94.6 ng/g dry wtRoche et al. (2007)
L-79Raibow trout3MuscleRae Lake (Sierra Nevada)1995, 1996USA1.24 ng/g wet wtOhyama et al. (2004)
L-80Raibow trout6MuscleBlue Lake (Sierra Nevada)1995, 1996USA2.13 ng/g wet wtOhyama et al. (2004)
L-81Raibow trout5MusclePear Lake (Sierra Nevada)1995, 1996USA9.99 ng/g wet wtOhyama et al. (2004)
L-82Raibow trout2MuscleDonner Lake (Sierra Nevada)1995, 1996USA3.71 ng/g wet wtOhyama et al. (2004)
L-83Raibow trout4MuscleHuntington Lake (Sierra Nevada)1995, 1996USA30.55 ng/g wet wtOhyama et al. (2004)
L-84Raibow trout5MuscleLake Berryessa (Sierra Nevada)1995, 1996USA13.01 ng/g wet wtOhyama et al. (2004)
L-85Lake trout10MuscleLake Chelan (Wapato Basin)2003USA943 ng/g wet wtWashington State Department of Ecology (2005)
L-86Burbot7MuscleLake Chelan (Wapato Basin)2003USA315 ng/g wet wt
L-87Kokanee7MuscleLake Chelan (Wapato Basin)2003USA57 ng/g wet wt
L-88Raibow trout3MuscleLake Chelan (Wapato Basin)2003USA14 ng/g wet wt
L-89Burbot3MuscleLake Chelan (Lucerne Basin)2003USA22 ng/g wet wt
L-90Raibow trout1MuscleRoses Lake2003USA96 ng/g wet wt
L-91Black Crappie1MuscleRoses Lake2003USA32 ng/g wet wt
L-92Lg Scale Sucker15MuscleVancouver Lake2005-2006USAND23 ng/g wet wtWashington State Department of Ecology (2007)
L-93Common Carp15MuscleVancouver Lake2006USAND65 ng/g wet wt
L-94Lg Mouth Bass5MuscleVancouver Lake2006USAND42 ng/g wet wt
L-95N. pikeminnow (Large size)10WholeLake Washington2001-2003USA258 ng/g wet wtMcIntyre & Beauchamp (2007)
L-96Cutthroat trout (Large size)10WholeLake Washington2001-2003USA168 ng/g wet wtMcIntyre & Beauchamp (2007)
L-97Yellow perch (Large size)9WholeLake Washington2001-2003USA59 ng/g wet wtMcIntyre & Beauchamp (2007)
L-98Smallmouth bass (Large size)3WholeLake Washington2001-2003USA63 ng/g wet wtMcIntyre & Beauchamp (2007)
L-99Lake trout10MuscleKusawa Lake1993Canada1.21 ng/g wet wt40.85 ng/g wet wtRyan et al. (2005)
L-100Lake trout14MuscleKusawa Lake1999Canada1.68 ng/g wet wt122.43 ng/g wet wtRyan et al. (2005)
L-101Lake trout9MuscleKusawa Lake2001Canada0.91 ng/g wet wt49.71 ng/g wet wtRyan et al. (2005)
L-102Lake trout10MuscleKusawa Lake2002Canada0.62 ng/g wet wt23.51 ng/g wet wtRyan et al. (2005)
L-103Lake trout24MuscleLake Laberge1993Canada4.69 ng/g wet wt360.87 ng/g wet wtRyan et al. (2005)
L-104Lake trout13MuscleLake Laberge1996Canada6.50 ng/g wet wt205.54 ng/g wet wtRyan et al. (2005)
L-105Lake trout5MuscleLake Laberge2000Canada2.30 ng/g wet wt82.96 ng/g wet wtRyan et al. (2005)
L-106Lake trout16MuscleLake Laberge2001Canada0.80 ng/g wet wt75.09 ng/g wet wtRyan et al. (2005)
L-107Lake trout5MuscleLake Laberge2002Canada1.58 ng/g wet wt43.56 ng/g wet wtRyan et al. (2005)
L-108Lake trout8MuscleLake Laberge2003Canada0.54 ng/g wet wt55.81 ng/g wet wtRyan et al. (2005)
L-109Trahira (Hoplias malabaricus)10MusclePonta Grossa Lake2005Brazil92.3 ng/g dry wtMiranda et al. (2008)
L-110Trahira (Hoplias malabaricus)10LiverPonta Grossa Lake2005Brazil54.68 ng/g dry wtMiranda et al. (2008)
L-111Japanese dace5MuscleLake Biwa2007Japan0.51 ng/g wet wt6.9 ng/g wet wtMinistry of the Environment, Japan (2009)
L-112Japanese dace5MuscleLake Biwa2008Japan0.68 ng/g wet wt8.0 ng/g wet wtMinistry of the Environment, Japan (2010)
L-113Japanese dace5MuscleLake Biwa2009Japan0.41 ng/g wet wt8.0 ng/g wet wtMinistry of the Environment, Japan (2011)
L-114Semutundu (Bagrus docmac)MuscleLake EdwardUnkownUganda33 ng/g wet wtSsebugere et al. (2009)
L-115Mamba (Protopterus aethiopinus)MuscleLake EdwardUnkownUganda29 ng/g wet wtSsebugere et al. (2009)
L-116Enjunguri (Haprochromis nigripinnis)MuscleLake EdwardUnkownUgandaNDSsebugere et al. (2009)
L-117Nile tilapia (Oreochromis niloticus)MuscleLake EdwardUnkownUganda33 ng/g wet wtSsebugere et al. (2009)
L-118Male (Clarias gariepinus)MuscleLake EdwardUnkownUgandaNDSsebugere et al. (2009)
L-119Tilapia and Catfish13Edible partLake Volta, Lake Bosumtwi, Weija Lake2008Ghana0.72 ng/g fat wt329.4 ng/g fat wtAdu-Kumi et al. (2010)
L-1206 kinds of fish60MuscleLakes (n=8) in Tibetan Plateau2006-2007China0.55 ng/g wet wt4.0 ng/g wet wt (+op')Yang et al. (2010)
L-121Common carp23UnknownBaiyangdian Lake2008China0.38 ng/g wet wt1.28 ng/g wet wtDai et al. (2011)
L-122Crucian carp25UnknownBaiyangdian Lake2008China0.47 ng/g wet wt1.03 ng/g wet wtDai et al. (2011)
L-123Crucian carp1MuscleLake Como2007Italy1.0 ng/g dry wt1.03 ng/g dry wt (+op')Villa et al. (2011)
L-124White fish1MuscleLake Como2007Italy7.35 ng/g dry wt12.4 ng/g dry wt (+op')Villa et al. (2011)
L-125Pike1MuscleLake Como2007Italy0.4 ng/g dry wt4.89 ng/g dry wt (+op')Villa et al. (2011)
L-126Chub1MuscleLake Como2007ItalyND5.89 ng/g dry wt (+op')Villa et al. (2011)
L-127Perch1MuscleLake Como2007Italy0.7 ng/g dry wt7.75 ng/g dry wt (+op')Villa et al. (2011)
L-128Pikeperch1MuscleLake Como2007Italy0.57 ng/g dry wt10.4 ng/g dry wt (+op')Villa et al. (2011)

Table 1.

Concentrations of T-HCH and T-DDT in fish from lakes in the world

No.SpeciesnaAnalyteRiverYearCountryT-HCH bT-DDT cReferences
R-1Color gudgeon10WholeGuanting Reservoir2002China7.15 ng/g wet wt9.23 ng/g wet wtSun et al. (2005)
R-2Feral carp10WholeGuanting Reservoir2002China0.72 ng/g wet wt5.04 ng/g wet wtSun et al. (2005)
R-3White fish1UnknownQiantang River (Downstream)2005China3.96 ng/g wet wt13.51 ng/g wet wtZhou et al. (2007)
R-4Crucian carp1UnknownQiantang River (Downstream)2005China3.84 ng/g wet wt5.64 ng/g wet wtZhou et al. (2007)
R-5Perch1UnknownQiantang River (Downstream)2005China2.62 ng/g wet wt8.34 ng/g wet wtZhou et al. (2007)
R-6Snake head mullet1UnknownQiantang River (Upstream)2005China3.18 ng/g wet wt5.01 ng/g wet wtZhou et al. (2007)
R-7Bulltrout1UnknownQiantang River (Upstream)2005China2.85 ng/g wet wt2.30 ng/g wet wtZhou et al. (2007)
R-8Ptychobarbus dipogon3MuscleLhasa River2005China0.286 ng/g wet wt2.07 ng/g wet wtYang et al. (2007)
R-9Schizopygopsis younhusbandi3MuscleLhasa River2005China0.75 ng/g wet wt2.99 ng/g wet wtYang et al. (2007)
R-10C. auratus5Edible partHuairou Reservoir (Beijing)2006China0.34 ng/g wet wt7.53 ng/g wet wtLi et al. (2008)
R-11M. anguillicauda-tus6Edible partHuairou Reservoir (Beijing)2006China5.42 ng/g wet wt44.17 ng/g wet wtLi et al. (2008)
R-12P. fulvidraco4Edible partHuairou Reservoir (Beijing)2006China1.93 ng/g wet wt34.5 ng/g wet wtLi et al. (2008)
R-13Crucian carp1Edible partQiantang River (Jinhua)2006China253 ng/g fat wt514 ng/g fat wtZhou et al. (2008)
R-14White fish1Edible partQiantang River (Jinhua)2006China222 ng/g fat wt315 ng/g fat wtZhou et al. (2008)
R-15Crucian carp1Edible partQiantang River (Fuchunjiang)2006China1054 ng/g fat wt1408 ng/g fat wtZhou et al. (2008)
R-16White fish1Edible partQiantang River (Fuchunjiang)2006China152 ng/g fat wt1330 ng/g fat wtZhou et al. (2008)
R-17Crucian carp1Edible partQiantang River (Fuyang)2006China577 ng/g fat wt155 ng/g fat wtZhou et al. (2008)
R-18White fish1Edible partQiantang River (Fuyang)2006China467 ng/g fat wt715 ng/g fat wtZhou et al. (2008)
R-19Crucian carp1Edible partQiantang River (Hangzhou)2006China936 ng/g fat wt1199 ng/g fat wtZhou et al. (2008)
R-20White fish1Edible partQiantang River (Hangzhou)2006China844 ng/g fat wt3008 ng/g fat wtZhou et al. (2008)
R-21Many kinds of fish19WholePearl River Estuary2004China0.20 ng/g wet wt*77 ng/g wet wt*Guo et al. (2008)
R-22Kissing gourami2WholeCiliwung River2003Indonesia24 ng/g fat wt800 ng/g fat wtSudaryanto et al. (2007)
R-23Common carp1WholeCiliwung River2003Indonesia3.4 ng/g fat wt37 ng/g fat wtSudaryanto et al. (2007)
R-24Tilapia mossambique1WholeCiliwung River2003Indonesia6.0 ng/g fat wt1100 ng/g fat wtSudaryanto et al. (2007)
R-25Walking catfish4WholeCiliwung River2003Indonesia11 ng/g fat wt610 ng/g fat wtSudaryanto et al. (2007)
R-26Unknown (n=10)UnknownRivers and streams in Kumaun Himalayas1999India1 ng/g wet wt13 ng/g wet wtSarkar et al. (2003)
R-27Scatophagus argus3MuscleFerok River2003India0.72 ng/g wet wt3.11 ng/g wet wtSarkar et al. (2006)
R-28Platicephalus sp.3MuscleKorappuzha River2003India5.4 ng/g wet wtNDSarkar et al. (2006)
R-29Etroplus suratensis3MusclePukatri River2003India0.06 ng/g wet wt0.44 ng/g wet wtSarkar et al. (2006)
R-30Burbot3LiverPechora River1988Russia11 ng/g wet wt57 ng/g wet wtZhulidov et al. (2002)
R-31Burbot3LiverPechora River1994Russia4 ng/g wet wt9 ng/g wet wtZhulidov et al. (2002)
R-32Several kinds103Edible partSava River2000Croatia0.70 ng/g wet wt*1.80 ng/g wet wt*Bosnir et al. (2007)
R-334 kinds of fish4MuscleDniester River (Upstream)2001Moldova17.3 ng/g wet wtSapozhnikova et al. (2005)
R-345 kinds of fish5MuscleDniester River (Downstream)2001Moldova10.2 ng/g wet wtSapozhnikova et al. (2005)
R-35European river lamprey31WholeRivers flowing (n=8) to Bothnian BayUnkownFinland3.03 ng/g wet wt46 ng/g wet wtMerivirta et al. (2006)
R-36European river lamprey19WholeRivers (n=5) flowing to Bothnian SeaUnkownFinland4.20 ng/g wet wt68 ng/g wet wtMerivirta et al. (2006)
R-37Chub3MuscleRiver Nestos (Paranesti)2004Greece0.27 ng/g wet wt0.40 ng/g wet wtChristoforidis et al. (2008)
R-38Chub3MuscleRiver Nestos (Komnina)2004Greece0.10 ng/g wet wtNDChristoforidis et al. (2008)
R-39Barbel3MuscleRiver Nestos (Paranesti)2004Greece0.91 ng/g wet wt0.47 ng/g wet wtChristoforidis et al. (2008)
R-40Barbel3MuscleRiver Nestos (Komnina)2004Greece0.15 ng/g wet wt0.25 ng/g wet wtChristoforidis et al. (2008)
R-41Common trout5MuscleRiver Turia2000Spain4.3 ng/g wet wtBordajandi et al. (2003)
R-42European eel11MuscleRiver Turia2000Spain45.3 ng/g wet wtBordajandi et al. (2003)
R-43Brown trout28WholeTwo rivers in Cantabria2001Spain0.55 ng/g dry wt20.2 ng/g dry wtGuitart et al. (2005)
R-44Eurasian minnow17WholeTwo rivers in Cantabria2001Spain1.04 ng/g dry wt23.0 ng/g dry wtGuitart et al. (2005)
R-45European eel16WholeTwo rivers in Cantabria2001Spain0.66 ng/g dry wt39.4 ng/g dry wtGuitart et al. (2005)
R-46Barbel3WholeEbro River Basin (Presa de Pina)2003Spain35.9 ng/g dry wtLacorte et al. (2006)
R-47Bleak6WholeEbro River Basin (Presa de Pina)2003Spain71.9 ng/g dry wtLacorte et al. (2006)
R-48Common carp1WholeEbro River Basin (Flix)2003Spain983 ng/g dry wtLacorte et al. (2006)
R-49Bleak3WholeEbro River Basin (Flix)2003Spain487 ng/g dry wtLacorte et al. (2006)
R-50Barbel2MuscleCinca River (Upstream)2002Spain31 ng/g wet wt (+op')De la Cal et al. (2008)
R-51Barbel2MuscleCinca River (Downstream)2002Spain780 ng/g wet wt (+op')De la Cal et al. (2008)
R-52Bleak1WholeCinca River (Upstream)2002Spain5 ng/g wet wt (+op')De la Cal et al. (2008)
R-53Bleak2WholeCinca River (Downstream)2002Spain508 ng/g wet wt (+op')De la Cal et al. (2008)
R-54Tilapia zilli2UnknownOgba RiverUnkownNigeria56 ng/g wet wtIze-Iyamu et al. (2007)
R-55Catfish2UnknownOgba RiverUnkownNigeria106 ng/g wet wtIze-Iyamu et al. (2007)
R-56Tilapia zilli2UnknownOvia RiverUnkownNigeria61 ng/g wet wtIze-Iyamu et al. (2007)
R-57Catfish2UnknownOvia RiverUnkownNigeria115 ng/g wet wtIze-Iyamu et al. (2007)
R-58Tilapia zilli2UnknownIkoro RiberUnkownNigeria20 ng/g wet wtIze-Iyamu et al. (2007)
R-59Catfish2UnknownIkoro RiberUnkownNigeria34 ng/g wet wtIze-Iyamu et al. (2007)
R-60Smallmouth bass3WholeWillamette River (Lower Superfund)2000USA (Oregon)< 8 ng/g wet wt320 ng/g wet wtSethajintanin et al. (2004)
R-61Common carp3WholeWillamette River (Lower Superfund)2000USA (Oregon)< 8 ng/g wet wt97 ng/g wet wtSethajintanin et al. (2004)
R-62Carp3MuscleOkanogan River (Oroville)2001USA336 ng/g wet wtWashington State Department of Ecology (2003)
R-63Mountain whitefish3MuscleOkanogan River (Oroville)2001USA350 ng/g wet wt
R-64Smallmouth bass3MuscleOkanogan River (Oroville)2001USA157 ng/g wet wt
R-65Akupa sleeper fish1UnknownHanalei River2001USA (Hawai'i)< 1 ng/g wet wt< 2 ng/g wet wtOrazio et al. (2007)
R-66Chinook salmonwholeLower Columbia Estuary2001-2002USA1800-27000 ng/g fat wt (+op')Johnson et al. (2007)
R-67Largemouth bass10wholeMobile River basin (Lavaca)2004USA (Alabama)24.9 ng/g wet wtHinck et al. (2009)
R-68Largemouth bass10wholeMobile River basin (Mcintosh)2004USA (Alabama)6946 ng/g wet wtHinck et al. (2009)
R-69Largemouth bass10wholeMobile River basin (Bucks)2004USA (Alabama)92.8 ng/g wet wtHinck et al. (2009)
R-70Largemouth bass8wholeMobile River basin2004USA53.84 ng/g wet wtHinck et al. (2008)
R-71Largemouth bass6wholeApalachicola-Chattahoochee-Flint River Basin2004USA87.45 ng/g wet wtHinck et al. (2008)
R-72Largemouth bass6wholeSavannah River Basin2004USA18.98 ng/g wet wtHinck et al. (2008)
R-73Largemouth bass6wholePee Dee River Basin2004USA37.84 ng/g wet wtHinck et al. (2008)
R-74Carp8wholeMobile River basin2004USA41.58 ng/g wet wtHinck et al. (2008)
R-75Carp6wholeApalachicola-Chattahoochee-Flint River Basin2004USA90.64 ng/g wet wtHinck et al. (2008)
R-76Carp6wholeSavannah River Basin2004USA16.42 ng/g wet wtHinck et al. (2008)
R-77Carp6wholePee Dee River Basin2004USA20.42 ng/g wet wtHinck et al. (2008)
R-78Chub10MuscleRiver Elbe (Downstream Pardubice)2004Czech Republic24 ng/g fat wt2850 ng/g fat wt (+op')Randak et al. (2009)
R-79Chub8MuscleRiver Elbe (Downstream Neratovice)2004Czech Republic486 ng/g fat wt4830 ng/g fat wt (+op')Randak et al. (2009)
R-80Chub4MuscleRiver Elbe (Downstream Usti nad Labem)2004Czech Republic53 ng/g fat wt6480 ng/g fat wt (+op')Randak et al. (2009)
R-81Chub (Leuciscus cephalus)10MuscleSvratka River (Modřice)Apr.-2007Czech Republic1.0 ng/g wet wt34.9 ng/g wet wt (+op')Lána et al. (2010)
R-82Chub (Leuciscus cephalus)10MuscleSvratka River (Modřice)Oct.-2007Czech Republic0.7 ng/g wet wt29.4 ng/g wet wt (+op')Lána et al. (2010)
R-83Chub (Leuciscus cephalus)9MuscleSvratka River (Rajhradice)Apr.-2007Czech Republic0.9 ng/g wet wt40.0 ng/g wet wt (+op')Lána et al. (2010)
R-84Chub (Leuciscus cephalus)11MuscleSvratka River (Rajhradice)Oct.-2007Czech Republic2.6 ng/g wet wt28.8 ng/g wet wt (+op')Lána et al. (2010)
R-85Fish (Large size)wholeMississippi River (Upper)2004-2005USA11.16 ng/g wet wtBlocksom et al. (2010)
R-86Fish (Large size)wholeMissouri River2004-2005USA8.18 ng/g wet wtBlocksom et al. (2010)
R-87Fish (Large size)wholeOhio River2004-2005USA18.32 ng/g wet wtBlocksom et al. (2010)
R-88Fish (Small size)wholeMississippi River (Upper)2004-2005USA6.57 ng/g wet wtBlocksom et al. (2010)
R-89Fish (Small size)wholeMissouri River2004-2005USA5.47 ng/g wet wtBlocksom et al. (2010)
R-90Fish (Small size)wholeOhio River2004-2005USA15.60 ng/g wet wtBlocksom et al. (2010)
R-91European eel30MuscleGarigliano River (Campania region)2005-2006Italy52.91 ng/g wet wtFerrante et al. (2010)
R-92Brown trout (Salmo trutta)9MuscleQuemquentreu river2006Argentina1.7 ng/g wet wtOndarza et al. (2011)
R-93Brown trout (Salmo trutta)9LiverQuemquentreu river2006Argentina7.4 ng/g wet wtOndarza et al. (2011)
R-94Sábalo fish (Prochilodus lineatus)7MuscleRío de la Plata basin2003-2004Argentina9 ng/g wet wt340 ng/g wet wt (+op')Colombo et al. (2011)
R-95Eel10MuscleRivers in South Canterbury2009New Zealand33.5 ng/g wet wt *Stewart et al. (2011)
R-96Brown trout5MuscleRivers in South Canterbury2009New Zealand16.8 ng/g wet wt *Stewart et al. (2011)
R-97Largemouth bassMuscleBlackwater River (Lower)2004USA (Florida)NDKarouna-Renier et al. (2011)
R-98Largemouth bassMusclePerdido River (Lower)2004USA (Florida)0.51 ng/g wet wtKarouna-Renier et al. (2011)
R-99Largemouth bassMuscleYellow River (Lower)2004USA (Florida)NDKarouna-Renier et al. (2011)
R-100Tilapia8MuscleNoha River (Okinawa-Manko)2006Japan24 ng/g fat wt3800 ng/g fat wtMalarvannan et al. (2011)
R-101Tilapia8MuscleHija River (Okinawa-Kadena )2006Japan4.7 ng/g fat wt1100 ng/g fat wtMalarvannan et al. (2011)
R-102Tilapia8MuscleShikaza River (Okinawa-Onna village)2005Japan10 ng/g fat wt680 ng/g fat wtMalarvannan et al. (2011)

Table 2.

Concentrations of T-HCH and T-DDT in fish from rivers in the world

Residue of T-DDT and T-HCH in fish from lakes in the world is shown in Figures 1 and 2, respectively, for the concentration data (ng/g wet wt.) and (ng/g fat wt. and ng/g dry wt. possible to be calculated as ng/g wet wt.). Each of the T-DDT and T-HCH concentration data was compared for the 38 lakes surveyed in 8 countries of Europe and America and 8 countries of Asia and Africa from 1995 to 2008. Each data is shown as single determination value (n=1) and mean (n≧2) or mean and range values (n≧2) for the surveys in plural fish species, sampling sites and survey years.

T-DDT concentrations in the fish from the lakes of America were relatively high and the higher concentrations were detected in USA like the previous report [102]. Those of Europe were relatively low except for two lakes in Italy. Those of Asia and Africa including Japan were relatively low as a whole, although relatively high concentrations were detected in a part of lakes in China. T-HCH concentrations in the fish from the lakes in the world were relatively low. The highest T-HCH concentration was 46 ng/g wet wt. in Taihu Lake of China [46] and relatively low concentration of 1.4 ng/g wet wt. (average, n=7) was detected in Lake Biwa of Japan [22-28].

Residue of T-DDT and T-HCH in fish from rivers in the world is shown in Figures 3 and 4, respectively, for the concentration data (ng/g wet wt.) and (ng/g fat wt. and ng/g dry wt. possible to be calculated as ng/g wet wt.). Each of the T-DDT and T-HCH concentration data was compared for the 28 rivers surveyed in 8 countries of Europe and America, 4 countries of Asia, Africa and Oceania from 2000 to 2009. Each data is shown as single determination value (n=1) and mean (n≧2) or mean and range values (n≧2) for the surveys in plural fish species, sampling sites and survey years.

Figure 1.

Residue of T-DDT in fish from lakes in the worl

Figure 2.

Residue of T-HCH in fish from lakes in the world

Figure 3.

Residue of T-DDT in fish from rivers in the world

Figure 4.

Residue of T-HCH in fish from rivers in the world

T-DDT concentrations in the fish from the rivers of USA were relatively high like the previous report [102]. Those of Europe were relatively low except for a part of lakes in Czech Republic and Spain. Those of Asia and Africa were relatively low as a whole, although relatively high concentrations were detected in a part of rivers of China.

T-HCH concentrations in the fish from the rivers in the world were relatively low like the lakes in the world and the highest T-HCH concentration was 7.7 ng/g wet wt. (average, n=8) in Qiantang River of China [101].

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3. Long-term trends of T-DDT and T-HCH in fish from lakes in the world

T-HCH and T-DDT concentrations in fish were calculated as the simple sum of the constituents. T-HCH is the sum of α-HCH, β-HCH and γ-HCH and T-DDT is the sum of pp’-DDT, pp’-DDD and pp’-DDE. For Japan, T-DDT and T-HCH concentration data in Japanese dace from Lake Biwa were cited from reports of Ministry of the Environment, Japan (1980 – 2011) [1-31]. For Canada and USA, T-DDT concentration data in lake trout from Lake Ontario and Lake Michigan were cited from a report of Environment Canada and U.S. Environmental Protection Agency (2007) [32] and a source figure of U.S. Environmental Protection Agency (2009) [33], respectively. For Sweden, T-DDT concentration data in pike from Lake Storvindeln were cited from a source figure of Swedish EPA (2002) [34].

All data were analyzed using Microsoft Excel graph wizard. For each location and analyte, nonlinear procedure was used to fit the exponential model: y=ae-kx, where y is the concentration in each composite sample, x is the sampling date, and a and k are model parameters estimated by nonlinear procedure to obtain a specific model that best fits the data.

Long-term trends of T-DDT and T-HCH in Japanese dace from Lake Biwa are shown from 1979 to 2009 in Figure 5 along with long-term trends estimated using the first-order model. Both insecticides were found to decline in a consistent pattern. Model parameters (a, k) and R2 values were calculated for each of the data sets and are shown in Figure 5. Half-lives (t1/2) were calculated for T-DDT and T-HCH from a parameter (k). The t1/2 values were 9 years for T-DDT and 4 years for T-HCH.

Long-term trends of T-DDT in fish from Lake Biwa, Lake Ontario, Lake Michigan and Lake Storvindeln are similarly shown in Figure 6. The t1/2 values of T-DDT were 9, 11, 8 and 7 years, respectively, in Lake Biwa, Lake Ontario, Lake Michigan and Lake Storvindeln. There were no wide differences in the t1/2 values of T-DDT in the fish among the four lakes. The same extent of the decline rate in the T-DDT inflow into the four lakes was presumed from the same extent of the decline rate of T-DDT in the fish of the four lakes.

Figure 5.

Long-term trends of T-DDT and T-HCH in Japanese dace from Lake Biwa

Figure 6.

Long-term trends of T-DDT in fish from Lake Biwa, Lake Ontario, Lake Michigan and Lake Storvindeln

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4. Composition of T-DDT and T-HCH in fish from lakes and rivers in the world

Composition of T-DDT in fish from lakes in the world is shown in Figure 7 for the survey data in the 25 lakes in 15 countries of Europe, America, Asia and Africa from 1996 to 2008 [22-28, 35, 39, 41, 42, 44, 47, 49-53, 55, 56, 58, 60, 61, 64, 65, 67, 68, 70]. Few (ND∼0.6 %) or low (1∼6 %) percentage of PP'-DDT was detected in Lake Biwa and Lake Mashu of Japan, Lake Tai and three lakes of China, Lake Stuorajavri of Norway, Lake Ganzirri of Italy and Sir Dam Lake of Turkey. Metabolites of PP'-DDT (pp'-DDE and pp'-DDD) were detected at high percentage and long-term no use of DDT was presumed in the countries. On the other hand, high percentage (44∼88 %) of PP'-DDT was detected in Lake Edward of Uganda, three lakes of Ghana, Lake Burullus of Egypt, Lake Victoria of Tanzania and Ponta Grossa Lake of Brazil. DDT was presumed to be used in the countries in recent years or in the sampling date. The use of organochlorine pesticids such as DDT was prohibited or restricted in the 1970’s for Japan and 1980’s for Europe and in 1983 for China. This corresponded well to the survey data described above. Low percentage of PP'-DDT in the fish from Lake Michigan and Lake Superior of USA was reported in the previous report [102]. The percentage of PP'-DDT was similarly low (5 %) in the fish from Vancouver Lake in the present report. In Africa, the use of DDT was restricted in in the 1980’s and low percentage of PP'-DDT was reported in the fish from Manzara Lake or Idku Lake in the previous report [102]. The present result in Lake Burullus was different from the previous report and the use of DDT was presumed in recent years or in the sampling date. Details of the restriction on the use of DDT in Egypt were obscure.

Composition of T-DDT in fish from rivers in the world is shown in Figure 8 for the survey data in the 16 rivers in 8 countries of Europe, America, Asia, Africa and Oceania from 2000 to 2009 [51, 68, 73, 77, 79, 80, 83, 86, 88, 91, 94, 95, 98, 100, 101].

In China, relatively high percentage (38 %) of PP'-DDT was detected in Qiantang River of China (2005). However, low percentage (2∼10 %) of PP'-DDT was detected in Lhasa River, Huairou Reservoir and Qiantang River (2006). In Japan, India, Greece, Spain and USA, low percentage (ND∼12 %) of PP'-DDT was similarly detected. No use of DDT was presumed in recent years or in the sampling date in all rivers except for Qiantang River of China surveyed in 2005.

Composition of T-HCH in fish from lakes in the world is shown in Figure 9 for the survey data in the 16 lakes in 8 countries of Europe, America, Asia and Africa from 1996 to 2008 [22-28, 35, 42, 44, 51, 53, 56, 58, 60, 61, 65, 68]. Composition of T-HC in Lake Biwa of Japan (α-HCH 7 %, β-HCH 91 % and γ-HCH 3 %) was similar to that in Lake Tai of China (α-HCH 10 %, β-HCH 84 % and γ-HCH 6 %). It was known that technical HCH (α-HCH 65∼70 %, β-HCH 6∼14 %, γ-HCH 10∼13 % andδ-HCH 5∼8 %) had been used in China, India and former Soviet Union since 1979 [103]. In Japan, technical HCH was also used without purification until 1971. This is the reason for the similarity of HCH composition in the fish between Japan and China (Lake Biwa and Lake Tai). However, the percentage of β-HCH in Yamdro Lake and Gaobeidian Lake was relatively low and the percentage of β-HCH in Lake Biwa of Japan was higher than that in the lakes of China. There was a probability of high β-HCH percentage in Japan because β-HCH was highly persistent and the period after prohibition on the use of β-HCH was longer in Japan than in China. On the other hand, the percentage of β-HCH in Rainbow trout and Japanese dace from Lake Mashu in Japan was low. Composition of T-HC in Japanese dace from Lake Mashu (α-HCH 64∼67 %, β-HCH 11 % and γ-HCH 22∼25 %) was much different from that of Lake Biwa (α-HCH 6∼8 %, β-HCH 89∼92 % and γ-HCH 2∼3 %). This is probably because HCH was loaded in Lake Mashu through the atmosphere [104] and the percentage of α-HCH in the water of Lake Mashu was much higher than that of Lake Biwa.

Figure 7.

Composition of T-DDT in fish from lakes in the world

Figure 8.

Composition of T-DDT in fish from rivers in the world

Figure 9.

Composition of T-HCH in fish from lakes in the world

On the other hand, purified lindane (γ-HCH: more than 99 %) was used in Europe and America differently from Japan, China, etc. This is probably because of the high percentage of γ-HCH in Bolsena Lake and Salto Lake of Italy, Sir Dam Lake of Turkey, Lake Burullus of Egypt, Lake Tanganyika of Burundi and three lakes of Ghana.

Composition of T-HCH in fish from rivers in the world is shown in Figure 10 for the survey data in the 11 rivers in 5 countries of Europe and Asia from 2001 to 2006 [51, 68, 73, 77, 86, 92, 100, 101].

In China, high percentage of γ-HCH was detected in Qiantang River and Huairou Reservoir differently from the survey data in the lakes. The use of lindane was presumed in the two river basins. In Korappuzha River of India, the use of technical HCH was presumed and this corresponded well to the report that technical HCH had been used in China, India and former Soviet Union since 1979 [103]. Particularly high percentage of γ-HCH was detected in Nestos River of Greece and this corresponded well to the use of lindane in Europe and America similarly in the case of the lake. For Okinawa Prefecture in Japan, the use of technical HCH in Shikaza River and Hija River and the use of lindane in Noha River were presumed from the composition of T-HCH shown in Figure 10. The high percentage of γ-HCH in Noha River did not correspond to the use of technical HCH in Japan.

Figure 10.

Composition of T-HCH in fish from rivers in the world

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5. Conclusion

T-DDT concentrations in the fish from the lakes and rivers of America were relatively high, but those of Europe, Asia and Africa were relatively low. T-HCH concentrations in the fish were relatively low in both of the lakes and rivers in all over the world. T-DDT and T-HCH compositions were respectively compared among lakes and rivers from America, Europe, Asia and Africa. DDT was presumed to be used in Uganda, Egypt, Tanzania and Brazil in recent years or in the sampling date from the high percentage of pp'­DDT in the composition of T-DDT and its metabolites in the several kinds of fish from Lake Edward, Lake Burullus, Lake Victoria and Ponta Grossa Lake. No use of DDT was presumed in USA and European countries from the low percentage of pp'­DDT in the lake fish in the countries. Technical HCH was presumed to be used in Japan, China and India from the low percentage of γ­HCH in the composition of T-HCH in the lake and the river fish in the countries. On the contrary, Lindane was presumed to be used in the countries of Europe and Africa from the high percentage of γ­HCH in the lake and the river fish in the countries. Half-lives (t1/2) of T-DDT in fish from lakes in Japan, Canada, USA and Sweden were calculated from the long-term monitoring data using an exponential decay model to evaluate the decline rate of DDT contamination in the lake environment. The t1/2 values were 9 years for Lake Biwa in Japan, 11 years for Lake Ontario in Canada, 8 years for Lake Michigan in USA and 7 years for Lake Storvindeln in Sweden. There were no wide differences in the t1/2 values of T-DDT in the fish among the four lakes.

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Written By

Taizo Tsuda

Submitted: 19 December 2011 Published: 01 August 2012