Ligninase-Mediated Removal of Natural and Synthetic Estrogens from Water: II. Reactions of 17β-Estradiol
Ligninase-Mediated Removal of Natural and Synthetic Estrogens from Water: II. Reactions of 17β-Estradiol
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DOI：
10.1021/es903058k
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发表时间：
2010-04-01
影响因子：
11.4
通讯作者：
Huang, Qingguo
中科院分区：
文献类型：
--
作者：
Mao, Liang;Lu, Junhe;Huang, Qingguo
我们在早期的工作中已经证明，一些天然和合成的雌激素可以通过木质素过氧化物酶（LiP）介导的反应有效转化。此类反应的行为受到天然有机物（NOM）和/或藜芦醇（VA）的存在的不同影响。某些白腐真菌，例如在 NOM 普遍存在的自然界中，黄孢原毛平革菌 (Phanerochaete chrysosporium) 产生 VA 作为次生代谢物以及 LIP。在此，我们报告了一项关于 LiP 介导的代表性雌激素 17 β-雌二醇 (E2) 氧化偶联反应产生的产物的研究，以及 NOM 和/或 VA 的存在如何影响产物的形成和分布。总共发现了六种产物，主要产物似乎是 E2 偶联产生的低聚物。我们的实验表明，这些产品可能在水中形成胶体固体，可以通过超滤去除或在超速离心过程中沉降。产品的这种胶体性质可能对其可处理性和环境运输产生重要影响。在 VA 存在下，产品往往会转向更高程度的低聚物。当反应体系中包含NOM时，E2和NOM之间似乎发生了交叉偶联。 E-SCREEN测试数据证实，通过LiP介导的连续反应可以有效消除E2的雌激素活性。
We have demonstrated in our earlier work that a few natural and synthetic estrogens can be effectively transformed through reactions mediated by lignin peroxidase (LiP). The behaviors of such reactions are variously influenced by the presence of natural organic matter (NOM) and/or veratryl alcohol (VA). Certain white rot fungi, e.g. Phanerochaete chrysosporium, produce VA as a secondary metabolite along with LIP in nature where NOM is ubiquitously present. Herein, we report a study on the products resulting from LiP-mediated oxidative coupling reactions of a representative estrogen, 17 beta-estradiol (E2), and how the presence of NOM and/or VA impacts the formation and distribution of the products. A total of six products were found, and the major products appeared to be oligomers resulting from E2 coupling. Our experiments revealed that these products likely formed colloidal solids in water that can be removed via ultrafiltration or settled during ultra centrifugation. Such a colloidal nature of the products could have important implications in their treatability and environmental transport In the presence of VA, the products tended to shift toward higher-degree of oligomers. When NOM was included in the reaction system, cross-coupling between E2 and NOM appeared to occur. Data obtained from E-SCREEN test confirmed that the estrogenicity of E2 can be effectively eliminated following sequential reactions mediated by LiP.