全氟辛酸(PFOA)及其醚羧酸替代品在菲律宾蛤仔体内的蓄积差异研究  

Accumulation Differences in Perfluorooctanoic Acid and Its Ether Carboxylic Acid Alternatives in the Manila Clam(Ruditapes philippinarum)

作　　者：秦翰林 毕宇杰 姜舒祺 吴成辰 谭志军[2] 耿倩倩 郭萌萌[2] QIN Hanlin;BI Yujie;JIANG Shuqi;WU Chengchen;TAN Zhijun;GENG Qianqian;GUO Mengmeng(College of Food Sciences&Technology,Shanghai Ocean University,Shanghai 201306,China;State Key Laboratory of Mariculture Biobreeding and Sustainable Goods,Yellow Sea Fisheries Research Institute,Chinese Academy of Fishery Sciences,Qingdao 266071,China)

机构地区：[1]上海海洋大学食品学院,上海201306 [2]海水养殖生物育种与可持续产出全国重点实验室、中国水产科学研究院黄海水产研究所,山东青岛266071

出　　处：《渔业科学进展》2025年第2期133-146,共14页Progress in Fishery Sciences

基　　金：现代农业产业技术体系专项资金(CARS-49);中国水产科学研究院基本科研业务费(2023TD76)共同资助。

摘　　要：以菲律宾蛤仔(Ruditapes philippinarum)为受试生物,研究了全氟辛酸(PFOA)及其醚羧酸替代品(HFPO-DA、HFPO-TA、HFPO-TeA)的生物富集、组织分布与消除规律以及机体蛋白质对目标物蓄积的影响。通过计算动力学参数,解析菲律宾蛤仔对PFOA及其醚羧酸替代品的富集、分布与消除行为。此外,通过提取菲律宾蛤仔体内水溶性蛋白,进行了体外蛋白质孵育实验,分析不同目标物与蛤仔机体蛋白质的结合率差异,并进一步通过分子对接技术,探讨了目标物分子–蛋白质之间的结合作用力及其与富集特征的相关性。结果表明,PFOA及其醚羧酸替代品在菲律宾蛤仔体内快速富集,富集速率按照HFPO-DA、PFOA、HFPO-TA、HFPO-TeA的顺序依次升高,在不同组织中的富集作用由强到弱依次为内脏团、鳃、外套膜、闭壳肌,并在净化21 d后趋于空白组水平。PFOA及其醚羧酸替代品在菲律宾蛤仔体内的蓄积能力、不同目标物分子–蛤仔机体蛋白质的结合率均与目标物浓度密切相关,浓度越低,吸收速率常数(Ku)和生物浓缩系数(BCF)越大,蛋白质结合率越低,其分子结构也是富集能力强弱和蛋白质结合力强弱的关键影响因素,C-O键和碳氟链的增加有助于目标物分子与蛋白质残基的碱基结合,目标物在各组织中的含量和蛋白结合率由低到高依次为HFPO-DA、PFOA、HFPO-TA、HFPO-TeA。使用分子对接技术进一步验证了4个目标物与脂肪酸结合蛋白FABP1-A之间的结合作用力,其结合能由低到高依次为HFPO-TeA、HFPO-TA、PFOA、HFPO-DA,结合能越低,越容易与蛋白质结合。目标物的极性端与FABP1-A氨基酸残基直接形成氢键,疏水端则与非极性残基有疏水相互作用,氢键作用与疏水相互作用共同促进了PFOA及其醚羧酸替代品与蛋白质的相互结合,氢键数量的多少是导致目标物与蛋白结合亲和力差异的重要原因。本研究结果有助于阐释双壳贝类中Perfluorooctanoic acid(PFOA)is a synthetic organic chemical with unique hydrophobic and oleophobic properties.It is extensively used in the production of a wide range of essential industrial and consumer products including aqueous film-forming foams,medical devices,and textiles.PFOA is widespread in aquatic environments and has attracted global attention due to the serious ecological risks it poses.Consequently,several countries and organizations have implemented strict restrictions or controls on its use.In 2019,PFOA and its salts were included as Annex A of the Stockholm Convention on Persistent Organic Pollutants,and in 2023,the Ministry of Ecology and Environment of the People's Republic of China and six other departments issued the"Key Regulated New Pollutant List 2023",which proposed environmental risk control measures for PFOA,its salts,and related compounds.With an increase in regulatory measures,the production and use of PFOA have declined,resulting in the rapid development and use of alternatives.Hexafluoropropylene oxide dimer acid(HFPO-DA),trimer acid(HFPO-TA),and tetramer acid(HFPO-TeA)—composed of CF2 or CF2O repeating units—have emerged as principal alternatives that maintain chemical properties similar to those of PFOA and are predominantly used in the manufacture of fluoropolymers and their processing aids.As filter-feeding organisms,bivalves are prolific and have a broad geographic distribution.They possess a marked capacity for accumulating organic contaminants,making them ideal indicators for monitoring pollution in marine environments and assessing the status of various marine ecosystems.Therefore,Manila clams(Ruditapes philippinarum)were used as the test organism in this study and exposed to two concentrations(2 ng/mL and 200 ng/mL)of PFOA and its alternatives—HFPO-DA,HFPO-TA,HFPO-TeA—within a mariculture setting.The purpose of this study was to analyze the tissue distribution,accumulation,and elimination patterns of these compounds in clams,and to evaluate differences in the accumul

关 键 词：全氟辛酸(PFOA) 醚羧酸替代品 菲律宾蛤仔 生物富集 蛋白质结合模式 

分 类 号：X503.2[环境科学与工程—环境工程]