Tunable Azacrown-Embedded Graphene Nanomeshes for Ion Sensing and Separation

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.