Metal complexes and free radical toxins produced by Pfiesteria piscicida
Metal complexes and free radical toxins produced by Pfiesteria piscicida
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DOI：
10.1021/es0617993
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发表时间：
2007-02-15
影响因子：
11.4
通讯作者：
Gelasco, Andrew K.
中科院分区：
文献类型：
--
作者：
Moeller, Peter D. R.;Beauchesne, Kevin R.;Gelasco, Andrew K.
含金属的有机毒素Pfiesteria piscicida产生的，其特征在于，第一次，从五个不同的仪器方法：核磁共振光谱（NMR），电感耦合等离子体质谱（ICP-MS），液相色谱粒子束辉光放电质谱（LC/PB-GDMS），电子顺磁共振光谱（EPR），和X-射线吸收光谱（XAS）得到的确证数据。含金属毒素的高毒性是由于金属介导的自由基产生。这种活性模式解释了Pfiesteria的毒性，以及先前报道的由于自由基种类的短暂性质而难以观察分子靶标。毒素在纯化形式下是高度不稳定的，在所有活性丧失之前仅维持活性2-5天。活性提取物中的多种毒素同系物在白色光、pH值变化和长时间加热的情况下也易于分解。这些研究结果代表了第一个正式的分离和表征的自由基形成有毒的有机连接的金属络合物分离的河口/海洋甲藻。这些发现增加了对金属在河口环境中与生物系统相互作用的积极作用的理解，以及它们与人类健康的联系和影响。
Metal-containing organic toxins produced by Pfiesteria piscicida were characterized, for the first time, by corroborating data obtained from five distinct instrumental methods: nuclear magnetic resonance spectroscopy (NMR), inductively coupled plasma mass spectrometry (ICP-MS), liquid chromatography particle beam glow discharge mass spectrometry (LC/PB-GDMS), electron paramagnetic resonance spectroscopy (EPR), and X-ray absorption spectroscopy (XAS). The high toxicity of the metal-containing toxins is due to metal-mediated free radical production. This mode of activity explains the toxicity of Pfiesteria, as well as previously reported difficulty in observing the molecular target, due to the ephemeral nature of radical species. The toxins are highly labile in purified form, maintaining activity for only 2-5 days before all activity is lost. The multiple toxin congeners in active extracts are also susceptible to decomposition in the presence of white light, pH variations, and prolonged heat. These findings represent the first formal isolation and characterization of a radical forming toxic organic-ligated metal complex isolated from estuarine/marine dinoflagellates. These findings add to an increased understanding regarding the active role of metals interacting with biological systems in the estuarine environment, as well as their links and implications to human health.