Abstract Graphene oxide (GO)-based membranes were fabricated by first immobilizing GO nanosheet using polydopamine (PDA) on the polyvinylidene fluoride (PVDF) substrate and then tuning the interlaminar spacing and properties by the different crosslinkers (i.e., ethylenediamine (EDA) or β-cyclodextrin functionalized EDA (β-CD-EDA)) to investigate rejection performance and mechanism of three pharmaceuticals. The d-spacings of EDA crosslinked membrane (PDA-GO/EDA) and β-CD-EDA crosslinked membrane (PDA-GO/β-CD-EDA) were determined to be 1.13 and 0.97 nm, respectively, which were much higher than that of PDA coated GO membrane (PDA-GO) of 0.78 nm. The moderate and even relatively low rejection ratio of the pharmaceuticals demonstrated that molecular sieving didn't contribute significantly to the pharmaceutical rejection as expected. In addition to molecular sieving, the electrostatic and chemical interactions from the active sites GO might play the significant and noticeable role on pharmaceutical rejection. When adsorption was not much higher in some scenarios (i.e., carbamazepine at all pH, sulfadiazine @ pH = 11 and propranolol @ pH = 3), it was plausible that conformation of GO nanosheets dramatically changed, which resulted in decrease of d-spacing and thus much higher rejection ratio. In contrast, when adsorption was much higher in some scenarios (sulfadiazine @ pH = 3, 7 and propranolol @ pH = 7, 11), the solubility in the membrane matrix increased and therefore the rejection ratio decreased. The disagreement demonstrated that more attention should be paid on the interactions between pharmaceutical and GO membranes, although the stability of the membrane was enhanced by crosslinking.

中文翻译：

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氧化石墨烯膜对药物的排斥：交联剂的作用和排斥机制

摘要 通过首先使用聚多巴胺 (PDA) 将 GO 纳米片固定在聚偏二氟乙烯 (PVDF) 基材上，然后通过不同的交联剂（即乙二胺 (EDA) 或 β -环糊精功能化 EDA (β-CD-EDA)) 以研究三种药物的排斥性能和机制。EDA 交联膜 (PDA-GO/EDA) 和 β-CD-EDA 交联膜 (PDA-GO/β-CD-EDA) 的 d-间距分别为 1.13 和 0.97 nm，远高于PDA 涂层的 GO 膜 (PDA-GO) 的波长为 0.78 nm。药物的中等甚至相对较低的排斥率表明分子筛对预期的药物排斥没有显着贡献。除了分子筛分之外，来自活性位点 GO 的静电和化学相互作用可能在药物排斥方面发挥重要而显着的作用。当在某些情况下（即，卡马西平在所有 pH 下，磺胺嘧啶 @ pH = 11 和心得安 @ pH = 3）吸附并不高时，GO 纳米片的构象发生显着变化是合理的，这导致 d-间距和因此更高的拒绝率。相反，当在某些情况下（磺胺嘧啶 @ pH = 3, 7 和心得安 @ pH = 7, 11）吸附量高得多时，膜基质中的溶解度增加，因此截留率降低。分歧表明应该更多地关注药物和GO膜之间的相互作用，