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The adsorption behavior and mechanism of perfluorochemicals on oxidized fluorinated graphene sheets supported on silica
Analytical Methods ( IF 2.7 ) Pub Date : 2017-11-06 00:00:00 , DOI: 10.1039/c7ay02070h
Fan Li 1, 2, 3, 4 , Weili Wei 2, 3, 4, 5 , Die Gao 4, 6, 7, 8 , Zhining Xia 1, 2, 3, 4, 5
Affiliation  

This is the first report on the fabrication of oxidized fluorinated graphene sheets supported on silica (OFG@silica) for the selective adsorption of perfluorochemicals (PFCs). To increase the affinity towards PFCs, oxidized fluorinated graphene (OFG) was grafted onto amino-terminated alkyl chain modified silica (NH2-silica), thus producing a mixed-mode material combining fluorophilicity and hydrophobic affinity with anion-exchange properties. The adsorption behavior and mechanism of OFG@silica towards PFCs were explored using a solid phase extraction (SPE) method. For demonstration, several organic analytes including perfluorinated fatty acids (PFFAs), aromatic analytes and fatty acids (FAs) were employed as adsorbates. By analysing the physicochemical properties of analytes, we found that the adsorption amount of analytes was negatively correlated with their molecular acidity coefficient (pKa) and positively correlated with their octanol–water distribution coefficient (log D) at pH 7, suggesting that the anion-exchange effect and hydrophobic affinity played a major role in adsorption. Moreover, compared with FAs, PFFAs exhibited a higher adsorption amount which benefited from fluorous–fluorous interactions between PFFAs and OFG@silica. These findings suggested that OFG@silica might be a potential adsorbent for the enrichment of PFCs.

中文翻译:

全氟化学品在二氧化硅上负载的氧化氟化石墨烯片材上的吸附行为和机理

这是有关在二氧化硅(OFG @ silica)上负载氧化的氟化石墨烯片材的制造的第一份报告,用于选择性吸附全氟化物(PFC)。为了增加对PFC的亲和力,将氧化氟化石墨烯(OFG)接枝到氨基末端烷基链改性的二氧化硅(NH 2-二氧化硅),从而生产出具有氟交换性和疏水亲和性并具有阴离子交换特性的混合模式材料。采用固相萃取(SPE)法研究了OFG @二氧化硅对PFCs的吸附行为和机理。为了证明这一点,将几种有机分析物包括全氟化脂肪酸(PFFA),芳香族分析物和脂肪酸(FAs)用作了吸附物。通过分析分析物的理化特性,我们发现分析物的吸附量与其分子酸度系数(p K a)呈负相关,与它们的辛醇-水分布系数呈正相关(log  D)在pH值为7时,表明阴离子交换作用和疏水亲和力在吸附中起主要作用。此外,与FAs相比,PFFAs表现出更高的吸附量,这得益于PFFAs与OFG @二氧化硅之间的氟-氟相互作用。这些发现表明,OFG @二氧化硅可能是富集PFC的潜在吸附剂。
更新日期:2017-11-22
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