School of Chemistry, Indian Institute of Science Education and Research , Thiruvananthapuram, Kerala 695016, India.
ACS Appl Mater Interfaces. 2017 Jan 11;9(1):999-1010. doi: 10.1021/acsami.6b10528. Epub 2016 Dec 20.
Remarkable selectivity with which crown ethers served as macrocyclic hosts for various guest species has led to numerous investigations on structure-specific interactions. Successful fabrication of graphene nanomeshes has opened up a plethora of avenues for sensing and separation applications. Embedding crown ether backbones in graphene frameworks can therefore be an interesting strategy for exploring the advantages offered by crown ether backbones, yet having the properties of graphene-based materials. Motivated by the recent success in fabrication of crown ether-based graphene nanopores, herein we investigate their performance toward ion sensing and separation using electronic structure methods. The effect of topology and electronic properties of the nanopore are probed by considering a series of oxygen-based and nitrogen-based graphene crown ethers (crown-n; n = 1-6). Our computations have revealed the excellent alkali ion binding properties of azacrown-based graphene nanomeshes over conventional oxygen crown-based graphene nanomeshes and normal crown ethers. Selectivity in ion transmission through the nanomeshes is demonstrated by employing graphene crown ethers [crown-n (n = 4-6)]. To the best of our knowledge, this article is the first report on azacrown-based graphene nanomeshes and their possible applications in ion sensing and separation, an aspect that we hope will be demonstrated in experiments soon.
冠醚作为各种客体物种的大环主体具有显著的选择性，这促使人们对结构特异性相互作用进行了大量研究。成功制备石墨烯纳米网开辟了众多用于传感和分离应用的途径。因此，将冠醚骨架嵌入石墨烯骨架中可能是探索冠醚骨架优势的一种有趣策略，同时具有基于石墨烯的材料的特性。受最近在基于冠醚的石墨烯纳米孔制备方面取得的成功的启发，本文采用电子结构方法研究了它们在离子传感和分离方面的性能。通过考虑一系列基于氧和氮的石墨烯冠醚（冠-n；n=1-6），研究了纳米孔的拓扑和电子性质的影响。我们的计算表明，氮杂冠醚基石墨烯纳米网对常规氧冠醚基石墨烯纳米网和普通冠醚具有优异的碱离子结合性能。通过使用石墨烯冠醚[crown-n（n=4-6）]证明了纳米网中离子传输的选择性。据我们所知，本文首次报道了氮杂冠醚基石墨烯纳米网及其在离子传感和分离中的可能应用，我们希望这一方面能尽快在实验中得到证实。
