Natural Sources and Microbial Transformation of Marine Halogenated Pollutants

项目摘要/摘要 天然多溴有机化合物，如羟化多溴联苯醚(OH-- BDES)和多溴吡咯(PBPs)最近已成为人类健康关注的化学物质。 这些人为卤化持久性有机污染物(POPs)的天然产物亲属是 广泛分布于整个海洋食物网，并在人类食用的海鲜来源中积累。 我们和其他人已经证明了6-OH-BDE-47(甲状腺激素受体)等羟基-BDEs 而多溴联苯并苯酚，如四溴吡咯(兰诺定受体)，是一种有效的毒素，因此对 人类。然而，许多根本的问题仍然是关于这些天然物质的来源范围 有机溴分子，这些化学物质如何进入和移动通过海洋食物网，无论是 气候的变化将影响它们的生产和积累，以及人类是多还是少 受天然卤代持久性有机污染物的影响，而不是它们的生色对应物。的最新发现 摩尔和艾伦实验室已经严格建立了微生物的遗传和生化基础 海洋细菌不同谱系中天然羟基-BDE分子的合成。然而，全球 这些多溴持久性有机污染物在海洋生物群中的分布和普遍存在不能完全解释 到目前为止已发现的来源，表明存在其他生物来源，并正在积极贡献OH- -BDE和MeO--海洋食物网中的BDE积累。这些信息对于更准确地 确定导致海水鱼体内自然积累多溴二苯醚的营养连接和相互转化 归根结底，人类饮食暴露的风险。在这个项目中，新的遗传和生化证据表明 将为海洋大型藻类建立多溴二苯醚分子的生物合成和生物转化 利用转录组分析，海洋生物栖息地中多溴二苯醚分子的明显但未确定的来源 再加上生化酶的特性。多溴联苯醚的其他微生物来源 综合分析鱼类和海洋哺乳动物的合成/转化 利用基因组和代谢综合方法结合实验的相关微生物群 用多溴二苯醚分子或生物合成底物改良的微生物组浓缩反应器。建议数 这项工作将由SiO WHO的摩尔(生物化学)和艾伦(基因组学)的实验室联合进行 在这些领域有良好的合作和联合指导的记录。

Project Summary/Abstract Natural polybrominated organic compounds such as hydroxylated polybrominated diphenyl ethers (OH-- BDEs) and polybrominated pyrroles (PBPs) have recently emerged as chemicals of human health concern. These natural product relatives of anthropogenic halogenated persistent organic pollutants (POPs) are widely distributed throughout the marine food web and accumulate in seafood sources consumed by humans. We and others have demonstrated that OH--BDEs such as 6--OH--BDE--47 (thyroid hormone receptor) and PBPs such as tetrabromopyrrole (ryanodine receptor) are potent toxins and thus pose a potential risk to humans. Many fundamental questions however remain about the extent of sources for these natural organobromine molecules, how these chemicals enter and move through the marine food web, whether changes in the climate will impact their production and accumulation, and whether humans are more or less impacted by natural halogenated POPs versus their anthopogentic counterparts. Recent discoveries by the Moore and Allen laboratories have rigorously established the genetic and biochemical basis for the microbial synthesis of natural OH--BDE molecules in diverse lineages of marine bacteria. However, the global distribution and ubiquity of these polybrominated POPs in marine biota cannot be fully explained by the sources discovered thus far, suggesting additional biogenic sources exist and are actively contributing to OH- -BDE and MeO--BDE accumulation in the marine food web. This information is critical to more accurately identify trophic connections and interconversions that lead to natural PBDE accumulation in marine fish and ultimately, human dietary exposure risks. In this project, new genetic and biochemical evidence for the biosynthesis and biotransformation of PBDE molecules will be established for marine macroalgae, a conspicuous but uncharacterized source of PBDE molecules in marine habitats, using transcriptome analysis coupled with biochemical enzyme characterization. Additional microbial sources for PBDE synthesis/transformation will be characterized by the comprehensive analysis of fish and marine-- mammal associated microbiomes using integrated genomic and metabolomic approaches combined with experimental microbiome enrichment reactors amended with PBDE molecules or biosynthetic substrates. The proposed work will be undertaken jointly by the laboratories of Moore (biochemistry) and Allen (genomics) at SIO who have a proven track record of collaboration and joint mentorship in these areas.