Eawag, Swiss Federal Institute of Aquatic Science and Technology , CH-8600 Dübendorf, Switzerland.
Institute of Biogeochemistry and Pollutant Dynamics, ETH Zürich , CH-8092 Zurich, Switzerland.
Environ Sci Technol. 2016 Jan 19;50(2):711-20. doi: 10.1021/acs.est.5b04169. Epub 2016 Jan 6.
Biogenic selenium (Se) emissions play a major role in the biogeochemical cycle of this essential micronutrient. Microalgae may be responsible for a large portion of these emissions via production of methylated Se compounds that volatilize into the atmosphere. However, the biochemical mechanisms underlying Se methylation in microalgae are poorly understood. Here, we study Se methylation by Chlamydomonas reinhardtii, a model freshwater alga, as a function of uptake and intracellular Se concentrations and present a biochemical model that quantitatively describes Se uptake and methylation. Both selenite and selenate, two major inorganic forms of Se, are readily internalized by C. reinhardtii, but selenite is accumulated around ten times more efficiently than selenate due to different membrane transporters. With either selenite or selenate as substrates, Se methylation was highly efficient (up to 89% of intracellular Se) and directly coupled to intracellular Se levels (R(2) > 0.92) over an intracellular concentration range exceeding an order of magnitude. At intracellular concentrations exceeding 10 mM, intracellular zerovalent Se was formed. The relationship between uptake, intracellular accumulation, and methylation was used by the biochemical model to successfully predict measured concentrations of methylated Se in natural waters. Therefore, biological Se methylation by microalgae could significantly contribute to environmental Se cycling.
生物成因的硒(Se)排放对这种必需微量元素的生物地球化学循环起着重要作用。通过产生挥发到大气中的甲基化硒化合物,微藻可能是这些排放的主要贡献者。然而,微藻中硒甲基化的生化机制还知之甚少。在这里,我们研究了莱茵衣藻(Chlamydomonas reinhardtii)的硒甲基化,莱茵衣藻是一种模式淡水藻类,作为摄取和细胞内硒浓度的函数,并提出了一个定量描述硒摄取和甲基化的生化模型。两种主要的无机硒形式,亚硒酸盐和硒酸盐,都很容易被莱茵衣藻内化,但由于不同的膜转运蛋白,亚硒酸盐的积累效率比硒酸盐高约 10 倍。无论是亚硒酸盐还是硒酸盐作为底物,硒甲基化的效率都很高(高达细胞内硒的 89%),并且与细胞内硒水平直接相关(R²>0.92),细胞内浓度范围超过一个数量级。在细胞内浓度超过 10 mM 时,细胞内形成零价硒。生化模型利用摄取、细胞内积累和甲基化之间的关系,成功预测了天然水中甲基化硒的实测浓度。因此,微藻的生物硒甲基化可能会对环境硒循环产生重大影响。