Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
Department of Civil and Environmental Engineering, University of Michigan, Ann Arbor, MI 48109, USA.
Sci Adv. 2017 May 31;3(5):e1700041. doi: 10.1126/sciadv.1700041. eCollection 2017 May.
Methylmercury (CHHg) is a potent neurotoxin produced by certain anaerobic microorganisms in natural environments. Although numerous studies have characterized the basis of mercury (Hg) methylation, no studies have examined CHHg degradation by methanotrophs, despite their ubiquitous presence in the environment. We report that some methanotrophs, such as OB3b, can take up and degrade CHHg rapidly, whereas others, such as Bath, can take up but not degrade CHHg. Demethylation by OB3b increases with increasing CHHg concentrations but was abolished in mutants deficient in the synthesis of methanobactin, a metal-binding compound used by some methanotrophs, such as OB3b. Furthermore, addition of methanol (>5 mM) as a competing one-carbon (C1) substrate inhibits demethylation, suggesting that CHHg degradation by methanotrophs may involve an initial bonding of CHHg by methanobactin followed by cleavage of the C-Hg bond in CHHg by the methanol dehydrogenase. This new demethylation pathway by methanotrophs indicates possible broader involvement of C1-metabolizing aerobes in the degradation and cycling of toxic CHHg in the environment.
甲基汞(CHHg)是一种由某些自然环境中的厌氧微生物产生的强效神经毒素。尽管已有大量研究对汞(Hg)甲基化的基础进行了描述,但尚无研究检测甲烷营养菌对 CHHg 的降解作用,尽管它们在环境中普遍存在。我们报告说,一些甲烷营养菌,如 OB3b,能够迅速摄取并降解 CHHg,而另一些甲烷营养菌,如 Bath,则只能摄取而不能降解 CHHg。OB3b 的去甲基化作用随着 CHHg 浓度的增加而增加,但在缺乏某些甲烷营养菌(如 OB3b)所使用的金属结合化合物甲烷菌素合成的突变体中,这种作用被废除。此外,添加甲醇(>5mM)作为竞争一碳(C1)底物会抑制去甲基化,这表明甲烷营养菌对 CHHg 的降解可能涉及甲烷菌素对 CHHg 的初始结合,然后通过甲醇脱氢酶裂解 CHHg 中的 C-Hg 键。这种甲烷营养菌的新的去甲基化途径表明,在环境中有毒 CHHg 的降解和循环过程中,可能有更多的 C1 代谢好氧菌参与其中。