结合高分辨质谱法、荧光光谱法及分子对接研究全氟化合物与白蛋白的相互作用
Interactions of perfluorinated compounds with serum albumins by high resolution mass spectrometry, fluorescence spectroscopy and molecular docking
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摘要: 本文结合电喷雾离子源-四极杆串联时间飞行高分辨质谱法（ESI-QTOF HRMS）、荧光光谱法（FL）以及分子对接（MD）实验手段，研究了全氟辛酸（PFOA）、全氟十二酸（PFDoA）与牛血清白蛋白（BSA）的相互作用机制.首先，采用HRMS方法检测到了PFOA、PFDoA与BSA结合物的分子量信息，证实了这两种污染物与BSA能形成稳定复合物；利用荧光光谱法证实了两种污染物对BSA的荧光猝灭为静态猝灭，进一步验证了PFOA、PFDoA与BSA之间复合物的形成，同时计算了两种污染物对BSA的结合常数和结合位点数，得出PFDoA与BSA的结合常数更高的结论，这一实验结果也与其他研究工作结果互为印证，即全氟化合物的C-F链长对其与生物分子的分配常数的正比关系.另外，使用分子对接研究手段进一步验证了PFOA、PFDoA与BSA的3个结合位点之间均存在相互作用，两种污染物的极性端与BSA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，氢键作用与疏水作用共同促进PFCs有机污染物与蛋白质的相互结合.Abstract: The binding interaction of perfluorooctanoic acid (PFOA) and perfluorododecanoic acid (PFDoA) with bovine serum albumin was investigated by using a combination method of high resolution mass spectrometry (HRMS), fluorescence spectroscopy (FL) and molecular docking (MD). The HRMS analysis revealed that PFOA and PFDoA molecules could bind to BSA and informed stable complexes. Furthermore, fluorescence spectroscopy data demonstrated that PFOA and PFDoA can effectively quench the fluorescence of BSA belongs to static quenching mechanism. The association constant between PFDoA and BSA was higher than that between PFOA and BSA. The result was consisted with published researches that the partition coefficients of PFCs between protein and water increased with increasing perfluoroalkyl chain length. The result of MD further suggests that PDOA and PFDoA might be bound to three sites of BSA through the hydrophobic interaction and hydrogen bond. The polar head of PFCs interacts with the amino acid residues of BSA by H-bond, and the hydrophobic tail of PFCs interacts with the nonpolar residues of BSA by hydrophobic force.
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Key words:
- high resolution mass spectrometry /
- fluorescence spectroscopy /
- molecular docking /
- PFCs /
- albumins
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