Fu Heyun, Wang Bingyu, Zhu Dongqiang, Zhou Zhicheng, Bao Shidong, Qu Xiaolei, Guo Yong, Ling Lan, Zheng Shourong, Duan Pu, Mao Jingdong, Schmidt-Rohr Klaus, Tao Shu, Alvarez Pedro J J
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Jiangsu 210023, China.
School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Jiangsu 210094, China.
Sci Adv. 2022 Jul 29;8(30):eabn4650. doi: 10.1126/sciadv.abn4650.
Selective binding of organic compounds is the cornerstone of many important industrial and pharmaceutical applications. Here, we achieved highly selective binding of aromatic compounds in aqueous solution and gas phase by oxygen-enriched graphene oxide (GO) nanosheets via a previously unknown mechanism based on size matching and polarity matching. Oxygen-containing functional groups (predominately epoxies and hydroxyls) on the nongraphitized aliphatic carbons of the basal plane of GO formed highly polar regions that encompass graphitic regions slightly larger than the benzene ring. This facilitated size match-based interactions between small apolar compounds and the isolated aromatic region of GO, resulting in high binding selectivity relative to larger apolar compounds. The interactions between the functional group(s) of polar aromatics and the epoxy/hydroxyl groups around the isolated aromatic region of GO enhanced binding selectivity relative to similar-sized apolar aromatics. These findings provide opportunities for precision separations and molecular recognition enabled by size/polarity match-based selectivity.
有机化合物的选择性结合是许多重要工业和制药应用的基石。在此，我们通过富氧氧化石墨烯（GO）纳米片在水溶液和气相中实现了对芳香族化合物的高度选择性结合，其基于一种前所未知的尺寸匹配和极性匹配机制。GO基面未石墨化脂肪族碳上的含氧官能团（主要是环氧基和羟基）形成了高度极性区域，这些区域包围着略大于苯环的石墨区域。这促进了小的非极性化合物与GO孤立芳香区域之间基于尺寸匹配的相互作用，相对于较大的非极性化合物产生了高结合选择性。极性芳香族化合物的官能团与GO孤立芳香区域周围的环氧基/羟基之间的相互作用相对于类似尺寸的非极性芳香族化合物增强了结合选择性。这些发现为基于尺寸/极性匹配选择性的精确分离和分子识别提供了机会。
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