High-Throughput 2D Heteroatom Graphene Bioelectronic Nanosculpture: A Combined Experimental and Theoretical Study

In this study, chemical vapor deposition-synthesized heteroatom graphene (HGr) bioelectronic interfaces have been developed for ultrafast, all-electronic detection and analysis of molecules by driving them through tiny holes - or atompores - in a thin lattice of the graphene sheet, including the efforts toward facilitating enhanced electrocatalytic and mapping electron transport activities. The presence of chlorine, nitrogen, and oxygen in the crystalline graphitic layers (<7) has been confirmed using Raman spectroscopy, X-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. We report a swift bioelectrocatalytic response to step-by-step additions of the substrate with the achievement of a steady current within a few seconds. The response limit was 2.07 μM with a dynamic range of sensing from 2.07 μM to 2.97 mM. The electronic properties and adsorption energies of hydroquinone and p-benzophenone molecule adsorption on pristine, O-, N-, and Cl-doped graphene nanosheet surfaces were systematically investigated using first-principles calculations. The results revealed that the adsorption capacity was improved upon doping graphene nanosheets with O, N, and Cl atoms. Hence, Cl-doped graphene nanosheets were shown as a promising adsorbent toward hydroquinone and p-benzophenone detection.