Environmental Research of naturally produced lipophilic halogenated compounds in Oceania

为了研究海洋环境中卤代联吡咯和溴代甲氧基二苯醚的来源，我们调查了日本沿海水域、东亚（菲律宾、台湾和香港）、密克罗尼西亚（关岛和帕劳）和大洋洲（澳大利亚、新西兰和大溪地）的海绵、海鱼、鲨鱼和集体搁浅的哺乳动物。经查明，分布在太平洋的主要持久性天然有机卤素产品为卤代1-甲基-1 '，2-联吡咯、1，1'-二甲基-2，2 '-联吡咯、甲氧基化四溴二苯醚、二甲氧基化四溴联苯。在日本母乳中（n=65），这些天然有机卤素的浓度与多溴联苯醚（PBDEs）相似。这些成分被发现广泛分布在日本沿海水域的海鱼中。这些化合物的膳食暴露被认为是通过食用海鱼。这些产品可能来自密克罗尼西亚的海绵，那里的一些海绵含有大量的多溴二苯醚类化合物。这些天然有机卤素的分布在地理上是不同的。在大洋洲（澳大利亚东部）的海洋鱼类中，氯代1-甲基-1 '，2-联吡咯含量丰富，而溴代1，1'-二甲基-2，2 '-联吡咯则分布于北方太平洋，尤其是日本沿海水域。天然多溴二苯醚类化合物广泛分布于太平洋沿岸，但这些化合物的生物放大潜力似乎因物种而异。本研究所述的天然持久性有机卤素需要进行食物链研究和毒理学评价。

In order to investigate the origin of halogenated bipyrroles and brominated methoxylated diphenyl ethers in marine environment, we surveyed marine sponge, marine fish, sharks and mass-stranded mammals collected in Japanese coastal water, East Asia (Philippines, Taiwan and Hong Kong), Micronesia (Guam and Palau) and Oceania (Australia, New Zealand and Tahiti). Major persistent natural organohalogen products distributed in the Pacific were identified as halogenated 1-methyl-1',2-bipyrroles, 1,1'-dimethy1-2,2'-bipyrroles, methoxylated tetrabromodiphenyl ethers, dimethoxylated tetrabromobiphenyl. In Japanese mother's milk (n=65), these natural organohalogens were present at similar concentrations to polybrominated diphenyl ethers (PBDEs). These components were found to be widely distributed in marine fish from the Japanese coastal water. The dietary exposure to these compounds was suggested to be via consumption of marine fish. These products may be originated from marine sponge in Micronesia, where some of sponges contained high amounts of PBDE-like compounds. The distribution of these natural organohalogens was geographically different. Chlorinated 1-methyl-1',2-bipyrroles were abundant in marine fish from Oceania (East of Australia), whereas brominated1,1'-dimethyl-2,2'-bipyrroles were localized in the northern Pacific, especially in the Japanese coastal water. Natural PBDE-like compounds were distributed widely in the Pacific coast, but the biomagnification potential of these compounds seemed to be species-specific. The food chain study and toxicological evaluation are needed for natural persistent organohalogens described in this study.