1] Center for Oceans and Human Health, Scripps Institution of Oceanography, University of California-San Diego, La Jolla, California, USA. [2].
1] Center for Marine Biotechnology and Biomedicine, Scripps Institution of Oceanography, University of California-San Diego, La Jolla, California, USA. [2].
Nat Chem Biol. 2014 Aug;10(8):640-7. doi: 10.1038/nchembio.1564. Epub 2014 Jun 29.
Polybrominated diphenyl ethers (PBDEs) and polybrominated bipyrroles are natural products that bioaccumulate in the marine food chain. PBDEs have attracted widespread attention because of their persistence in the environment and potential toxicity to humans. However, the natural origins of PBDE biosynthesis are not known. Here we report marine bacteria as producers of PBDEs and establish a genetic and molecular foundation for their production that unifies paradigms for the elaboration of bromophenols and bromopyrroles abundant in marine biota. We provide biochemical evidence of marine brominases revealing decarboxylative-halogenation enzymology previously unknown among halogenating enzymes. Biosynthetic motifs discovered in our study were used to mine sequence databases to discover unrealized marine bacterial producers of organobromine compounds.
多溴二苯醚（PBDEs）和多溴联吡咯是在海洋食物链中生物累积的天然产物。由于其在环境中的持久性和对人类的潜在毒性，PBDEs 引起了广泛的关注。然而，PBDE 生物合成的天然来源尚不清楚。在这里，我们报告海洋细菌是 PBDEs 的生产者，并为其生产建立了遗传和分子基础，这统一了海洋生物中丰富的溴酚和溴吡咯的生物合成模式。我们提供了海洋溴化酶的生化证据，揭示了以前在卤化酶中未知的脱羧卤化酶学。在我们的研究中发现的生物合成基序被用于挖掘序列数据库，以发现未被发现的海洋细菌有机溴化合物的生产者。
