Chikyukagaku Geochemistry Distribution of mercury in ecosystems of Yambaru, northern part of Okinawa Island, Japan and its relat

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1 Chikyukagaku Geochemistry Distribution of mercury in ecosystems of Yambaru, northern part of Okinawa Island, Japan and its relationships with other elements Izumi WATANABE,TaichiAKIYAMA and Syoichi SANO Graduate School of Agriculture, Tokyo University of Agriculture and Technology Saiwai-cho, Fuchu, Tokyo , Japan Relatively high levels of Hg were found in the bodies of low tropic animals inhabiting Yambaru area when compared with unpolluted ecosystems. Especially, large centipede species which are the strong carnivore of invertebrates accumulated Hg with high concentration due to their high tropic in food web. In the same way, some species of raptors and carnivorous snake inhabiting forest accumulated Hg in their bodies. These facts supported that biomagnification of Hg exists in the ecosystem of Yambaru area. Interestingly, rare animals in the Yambaru area such as Anderson s crocodile newt as amphibians, Okinawa woodpecker, Ryukyu robin, and Okinawa rail as birds accumulated Hg with higher levels when compared with other animals niching at the same tropic levels. From analysis of inter-elemental relationships using concentration data of 25 trace elements in the animal bodies collected from Yambaru area, three toxic elements (lead, cadmium, and silver), five essential elements (selenium, chromium, vanadium, nickel, and cobalt), and one trace element (strontium) were correlated with Hg in the various animal groups such as invertebrate, amphibians, reptilian, omnivorous birds, carnivorous birds, omnivorous mammals, and carnivorous mammals. Key words: mercury,yambaru, biomagnifications, ecosystem, rare species ; 2003 Hg Se Horai et al., 2006; 2008 Hg Hg

2 Hg Hg UNEP, 2002 Hg Hg UNEP, 2002 V As Hg Hg 42 Hg Jaffe et al., 2005; 2007Hg Hg Hg Hg 25 Hg Hg Se 2002; Horai et al., 2006 Pb As Se V Hg Hg 10 Meghimatium sp. 4 Satsuma mercatoria atrata Geothelphusa grandiovvata Naruse 2 Chilopoda 3 Araneae 2 Cardiodactylus novaeguineae 5 Calliphara nobilis 5 Trypoxylus 2 5 Polypedates leucomystax 1 Rana narina 4 Rana okinavana 3 Buergeria japonica 1 Tylototriton andersoni 7 7 Hemidactylus frenatus 5 Trachemys scripta elegans 2 Dinodon semicarinatus 3 Amphiesma pryeri 4 Cyclophiops semicarinatus 3 Ovophis okinavensis 1 Hemibungarus japonicus boettgeri 123: Calonectris leucomelas 1 Butorides striatus 1 Bubulcus ibis 1 Scolopax rusticola 1 Scolopax mira 1 Porzana fusca 1 Amauronis phoenicurus 2 Gallinula chliropus 3 Columba janthina 1 Otus elegans 1 Otus lempiji 3 Ninox scutulata 3 Halcyon coromanda 2 Alcedo atthis 2 Dendrocopos kizuki 1 Hirundo rustica 1 Pycnonotus sinensis 1 Turdus pallidus 3 Cettia diphone 3 Zosterops japonica 2 Gallirallus okinawae 10 Sapheopipo noguchii 6 Erithacus komadori 10 6 Pteropus dasymallus inopinatus 4 Rhinolophidae pumilus 3

3 Diplothrix legatsu 5 Crocidura horsfieldii watasei 3 Rattus rattus 3 Herpestes auropunctatus 49 Mustela itatsi 30 Pentalagus furnessi 21 Tokudaia osimensis osimensis 2 Nycticorax nycticorax 1 S. mira 3 H. coromanda 1 A. atthis 1 Hypsipetes amaurotis 1 Corvus macrorhynchos 3 6 O. okinavensis C C g PFA 2.0 ml PFA PTFE g HG- 300 ICP-MS 4500 a, Agilent 25 7 Li 24 Mg 43 Ca 51 V 52 Cr 55 Mn 57 Fe 59 Co 60 Ni 63 Cu 66 Zn 69 Ga 75 As 82 Se 85 Rb 88 Sr 95 Mo 107 Ag 111 Cd 115 In 121 Sb 133 Cs 137 Ba 205 Tl 208 Pb SPSS ver for Mac. 2 Spearman Mann-Whitney U- test Turkey Hg Table 1 2 Hg Hg 22 g/g DW 15 g/g DW 3.1 g/g DW Hg 1.9 g/g DW Hg 1.6 g/g DW 2.6 g/g DW 1.7 g/g DW 5.3 g/g DW 3.5 g/g DW 4.8 g/g DW Table 3 Hg Hg Table 4 Hg 1.2 g/g DW: 0.99 g/g DW: 1.2 g/g DW: 1.0 g/g DW Hg Hg Hg 28 g/g DW6.2

Table 1 Average concentrations of trace elements in whole body of

4 渡邉泉秋山太 Table 2 Average concentrations of trace elements in the amphibia collected from Yambaru area (μg/g dry weight). Table 1 Average concentrations of trace elements in whole body of invertebrate collected from Yambaru area (μg/g dry weight). 32 一佐野翔一

5 沖縄島北部やんばる地域の生態系における水銀分布と他元素との関係 33 μg/g DW ハシブトガラス最高5.5μg/g DW といった肉食性の種に加えノグチゲラ最高7.6μg/g DW: 国指定特別天然記念物および国内希少野生動植物種アカヒゲで最高3.7μg/g DW という比較的 Table 3 Average concentrations of trace elements in the reptilians collected from Yambaru area (µg/g dry weight). 高い Hg 濃度が認められた肝臓中の Hg 解毒に関係すると考えられている Se 渡辺 2002; Horai et al., 2008 は Hg の蓄積傾向と類似した分布を示しオオミズナギドリやササゴイカワセミハシブトガラスといった魚食性の種に加えヤマシギアマミヤマシギヤンバルクイナアカヒゲといった山林生の希少種に10μg/g DW を超える高濃度がみられたここで爬虫類ではミミズ食のリュウキュウアオヘビに最高濃度が検出されており最高23μg/g DW 山林生の鳥類でみられた Se Hg 蓄積にはとくに土壌からの Se 供給といった点でミミズ類種未同定で最高22.1μg/g DW を鍵種とする食物網の寄与が示唆された無機 Hg の標的器官である腎臓の Hg 濃度も肝臓筋肉と同じくオオミズナギドリゴイサギササゴイオオコノハズクアカショウビンカワセミハシブトガラスといった魚食性の種に高濃度でやはりヤマシギアマミヤマシギヤンバルクイナアカヒゲシロハラといった山林生の希少種と爬虫類のガラスヒバァリュウキュウアオヘビヒメハブにも2 μg/g DW を超える比較的高い Hg 濃度がみられた Se 濃度はオオミズナギドリにくわえアマミヤマシギアカヒゲといった山林生の希少種に30μg/g DW を超えるレベルがみられた高次生物への Se の供給という視点から筋肉の Se 濃度に着目するとアマミヤマシギヤンバルクイナカラスバトノグチゲラアカヒゲシロハラといった希少種を含むグループが5μg/g DW を超える高濃度を示したまたオオミズナギドリカワセミといった魚食性種も高濃度であった爬虫類ではミシシッピアカミミガメアカマタガラスヒバァの筋肉中 Se 濃度が高かった Se は各種製品の材料として広く使用され化石燃料の燃焼からの発生も指摘されるがその年間総生産量は比較的小さい National Research Council, 1978 ガラス工場など局所的な汚染は知られるがとくにやんばる地域で大規模の発生源は考えられないことから天然由来の供給と考えられるつまり各動物はそれぞれの Hg 負荷に応じて食物から必須元素 Se を吸収率を変化させる等して補っていると考えられた

6 Table 4 Average concentrations of trace elements in the birds collected from Yambaru area ( g/g dry weight). Table 5 Hg Turkey p 0.05 Hg

7 Table 5 Average concentrations of trace elements in the mammals collected from Yambaru area (μg/g dry weight). 沖縄島北部やんばる地域の生態系における水銀分布と他元素との関係 35

8 IB Hg Hg Myotis mystacinus Myotis nattereri 2 Hg Cd Pb Hg 3.0 g/g DW Myotis mystacinuscd 6.27 g/g DW Myotis nattereripb 4.05 g/g DW Myotis mystacinus Walker et al., 2007 Hg Cd Pb Hg 2010 Hg 300 g/g DW 2 6g 21.8 mg Hg Hg 0.66 g/g DW 1.9 g/g DW Cristol et al., 2008: 0.05 g/g DW: g/g DW Hg 4 Hg 25 g/g DW Hg Conover and Vest, 2009 Se Hg Se Hg Hg Hg Hg Hg Hg Hg Hg Hg Fig

9 Fig. 1 Schematic model of Hg dynamics (biomagnification) in the ecosystem of Yambaru area, Okinawa, Japan. Arrows indicate prey-predator relationships. Hg Hg Hg Hg 2004 Watanabe et al., 1996

10 Hg Hg 1 g/g DW Hg 2009 Hg Hg Hg Li V Cs Co Ni Mo Pb Ga Cd Ag 10 Fig. 2 Table 6 Mn Cu Se Sr Ba Cr 6 Mo Cd Ag V Ga Co Pb Ni 8 V Pb Ni Co Ga Cs Li Tl In Ag 10 Hg Se Hg Cr Rb Ga Co Ni V Mo Pb Cd Ag 10 Li Ag Co Mo V Pb 6 Hg Hg V Se Ni Co Cd Pb Ag Ga Ba Elemtnts forming a same cluster with Hg Fig. 2 Dendrogram for trace elements concentrations in the bodies of invertebrates collected from Yambaru area, Okinawa, Japan by a result of cluster analysis.

Table 6 The list of elements forming same clusters with Hg using 26 analyzed element data Se Hg Hg Horai et al., 2006 Se Hg 60 g/g DW 1: 1 Se 24 g/g DW Hg Se Hg Hg 0.58 g/g DW Hg Se Hg Fig.

11 Table 6 The list of elements forming same clusters with Hg using 26 analyzed element data Se Hg Hg Horai et al., 2006 Se Hg 60 g/g DW 1: 1 Se 24 g/g DW Hg Se Hg Hg 0.58 g/g DW Hg Se Hg Fig. 2 Table 1 2 Se Hg Hg V Ga In Ba Hg p 0.05 Spearman Hg Ga Ba Cu Zn Co Ni p 0.05 Co p 0.05Se p 0.01 Mo p 0.05V Co Se p 0.01 Hg Sr Ba V 3 Cr Cu Rb Sr Mn Se V Ba 8 Table 6 12 Cr V Sr Cd Mo 5 Cr Se Mn V Sr 5 9 V Cr Cd Sr 4 Mn Se V Cr Sr 5 Hg Se V Cr Mn Cd Sr Table 6 Cd 10 g/g DW Sr Hg

12 Hg Se Hg V Sr Co 3 Cd Mn Cd Pb Se Rb Cu 6 Cu Rb Sr Zn Mn 5 Fig. 3 3 Hg Cd Pb Cd Pb Hg Hg 4 3 Hg Hg Hg Hg Hg Hg Fig Sr,Ba,Cd,Co,Pb Mo,Co,V,Ni,Ba,As Ni, Cs, Pb Mn,Rb,Cu,Se Mn,Se,Sr,Cr,Cu Cr,Mn,Se,Cu,Rb Mn,Rb,Cu,Sr,Pb,Cd,Cr,Se,Mo Cr,Cu,Rb,Mn,Se,Sr Fig. 3 Dendrograms indicate relationships among trace element concentrations in liver of three rare birds species from Yambaru area, Okinawa, Japan by results of cluster analysis.

13 Fig. 4 Dendrograms indicate relationships among trace element concentrations in liver of three mammal species from Nansei Islands, Japan by results of cluster analysis. Cu,Rb,Se,Cr,Mn,Cd,Sr,Mo,Pb,Co Cd,Co,Pb,Cs As,V,Ni,Co,Ba Mn,Cu,Rb,Ba,Cr,Sr,Se,Cd Hg Hg Se Se Cu Mn Fig. 4 Cr Rb Sr Pb Cd Ag As Hg Pb Cd As 25 Hg Pb Cd Ag Se Cr V Ni Co Table 6: As 2007 Hg Hg Se Cd Cr Sr Hg Pb Ag Co Ni Hg V Hg Spearman

14 Hg Hg Hg Hg Cd RF-085 RF-0908 Conover, M. R. and Vest, J. L. (2009) Selenium and mercury concentrations in California gulls breeding on the Great Salt Lake, Utah, USA. Environmental Toxicology and Chemistry, 28, Cristol,D.A.,Brasso,R.L.,Condon,A.M.,Fovargue,R.E., Friedman, S. L., Hallinger, K. K., Monroe, A. P. and White, A. E. (2008) The movement of aquatic mercury through terrestrial food webs. Science, 320, 335. Horai, S., Minagawa, M., Ozaki, H., Watanabe, I., Takeda, Y., Yamada,K.,Ando,T.,Akiba,S.,Abe,S.andKuno,K. (2006) Accumulation of Hg and other heavy metals in the Javan mongoose (Herpestes javanicus) captured on Amamioshima Island, Japan. Chemosphere, 65, Horai, S., Furukawa, T., Ando, T., Akiba, S., Takeda, Y., Yamada, K., Kuno, K., Abe, S. and Watanabe, I. (2008) Subcellular distribution and potential detoxification mechanisms of mercury in the liver of the Javan mongoose (Herpestes javanicus) in Amamioshima Island, Japan. Environmental Toxicology and Chemistry, 27, Jaffe, D., Prestbo, E., Swartzendruber, P., Weiss-Penzias, P., Kato, S., Takami, A., Hatakeyama, S. and Kajii, Y. (2005) Export of atmospheric mercury from Asia. Atmospheric Environment, 39, Herpestes javanicus National Research Council pp United Nations Environment Programme (UNEP) (2002) UNEP Global Mercury Assessment Summary of the Report. Walker,L.A.,Simpson,V.R.,Rockett,L.,Wienburg,C.L. and Shore, R. F. (2007) Heavy metal contamination in bats in Britain. Environmental Pollution, 148, Herpestes auropunctatus Watanabe, I., Ichihashi, H., Tanabe, S., Amano, M., Miyazaki, N., Petrov, E. A. and Tatsukawa, R. (1996) Trace element accumulation in Baikal seal (Phoca sibirica) from the Lake Baikal. Environmental Pollution, 94,

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<8CF6955C977095F18D908F912D E786477> 2.1.1.3 生態系 2.1.1.3.1 注目種 : 鳥類 (1) 調査目的本調査は慶佐次川とその周辺地域における鳥類の生息状況の把握を目的とする (2) 調査方法調査方法を表 2.1.1.3.1-1 に示すまた確認種における重要種の選定基準については表 2.1.1.3.1-2 の選定基準に従って重要な種の抽出を行ったなお使用した基準文献のカテゴリー等を表 2.1.1.3.1-3~4