抗污损活性物质丁烯酸内酯在靶标和非靶标海洋生物中的分子靶点及对非靶标物种潜在的环境危害评估

Biofouling increases the weight, drag, and surface corrosion of vessels and block drainage pipelines, leading to substantially increased maintenance costs and huge economic losses to maritime industries. In the past, toxic antifouling compounds such as tributyltin (TBT) were added to marine paints to control biofouling. However, the devastating environmental impact of toxic antifouling compounds led to the prohibition of their use. There is an urgent need for environmentally friendly antifouling compounds and many natural marine products have been identified as potential candidates for antifouling compounds. However, the modes of actions of most candidate compounds unknown and thus, it is not sure if these so-called environmentally friendly compounds will be really safer than the existing antifouling compounds. We recently developed a promising low-toxic antifouling butenolide with very low acute toxicity against both target and non-target organisms, including micro-algae, crustaceans, and fish. Chronic exposure of marine medaka (Oryzias melastigma), to butenolide also showed the lower toxicity indicated by multiple sensitive biomarkers, increased energy production from lipid oxidation for activated detoxification and faster recovery from the toxic effects than a very popular antifouling compound SeaNine 211 (4,5-dichloro-2-n-octyl-4-isothiazolin-3-one, DCOIT) which mainly disrupted the endocrine homeostasis and tended to be an potent estrogenic mimic. Furthermore, we identified a thiolase as the potential binding target of the butenolide in one of the major fouling species Balanus amphitrite. We raised our hypothesis that the butenolide causes energy shortage in fouling organisms so that they cannot complete larval settlement and metamorphosis, an energy demanding process. The objectives of the present proposal are:..1. To verify butenolide targets lipid oxidation in the target species Balanus amphitrite by characterization the interaction between the butenolide and the thiolase using Top-down and Bottom-up proteomic analysis;..2. To study the effect of butenolide and DCOIT on steroidogenic pathway in the non-target species O. melastigma using comparative proteomics and transcriptomics;..3. To evaluate the bioaccumulative potential and metabolic kinetics of the butenolide and DCOIT in the non-target species O. melastigma...We anticipate that our results will further demonstrate the effectiveness and environmental safety of the butenolide; enable us to compare the effect and molecular targets of the butenolide and DCOIT in both the target and non-target species; more importantly, if our hypothesis is correct, a new screening platform targeting the lipid oxidation of larvae may be established to search for more environmentally friendly antifouling compounds.

生物污损会增加船体自重和阻力，加快表面的腐蚀和堵塞进水管，给海洋产业带来巨大经济损失。有机锡抗污损涂料因其环境毒性已被禁用，我们亟需从海洋天然产物中寻找环境无害而高效的抗污损涂料。然而由于化合物活性机制未明，无法肯定它们就比现有的防污剂更安全有效。我们开发出高效低毒的防污化合物butenolide。它对靶标及非靶标生物毒性比DCOIT低，抑制作用可逆，在靶标生物中的作用靶点为thiolase，我们推断它通过干扰幼虫附着变态所需的能量代谢起作用。我们将运用BOTTOM-UP和TOP-DOWN分析来证明它对藤壶脂质氧化的作用; 应用蛋白质组学和转录组方法研究它和DCOIT对青鳉鱼类固醇代谢途径的影响; 评估它和DCOIT在青鳉鱼体内的生物积累性和代谢。通过比较它和DCOIT对靶标及非靶标生物的活性及其作用靶点验证它的高效低毒；并建立以幼虫脂质氧化为参照的环境友好防污损化合物筛选新方法。

生物污损会增加船体自重和阻力，加快表面的腐蚀和堵塞进水管，给海洋产业带来巨大经济损失。有机锡抗污损涂料因其环境毒性已被禁用，我们亟需从海洋天然产物中寻找环境无害而高效的抗污损涂料。然而由于化合物活性机制未明，无法肯定它们就比现有的防污剂更安全有效。我们前期开发出高效低毒的防污化合物butenolide，该化合物具有高效、对靶标及非靶标生物毒性比DCOIT低，抑制作用可逆等优点。本课题继续延续对丁烯酸内酯的研究，以DCOIT为阳性对照，主要对其在环境中的生物降解及对非靶标生物的作用机理及毒性风险进行详细的研究，从而评价其生态环境风险。本项目取得了一系列重要的研究成果：1）在目标物种生物膜中，通过多组学分析丁烯酸内酯对生物膜形成抑制作用机理。 2）应用蛋白质组学和转录组方法研究丁烯酸内酯以及其参照物DCOIT对非目标物种海洋青鳉鱼Oryzias melastigma的脂质氧化和其他的能量代谢途径的影响。3） 评估丁烯酸内酯对非目标物种海洋青鳉鱼的环境毒性风险，建立一套完整的防污剂的环境风险评估体系，这一套环境风险评估体系的建立，对以后抗污损活性物质的商品化过程具有显著指导意义。本项目根据研究目标和计划开展了大量的研究工作，于执行期间已在Env Sci Tech、ACS Sustainable Chemistry & Engineering、Biofouling等杂志发表了10篇SCI论文、取得的研究成果建立已丁烯酸内酯为标准的抗污损活性物质的生态风险评价平台。

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