Elucidating the effects of oxygen- and nitrogen-containing functional groups in graphene nanomaterials for applied electrochemistry by density functional theory

Graphene nanomaterials functionalized with oxygen groups [graphene oxide (GO) and reduced GO (rGO)] are either doped element nitrogen or nitrogen-containing aromatic moieties followed by the investigation of electrochemical properties that generally show enhanced electroanalytical performance. We studied structural, morphological, physical–chemical using correlative techniques. While we attribute their improved promoted simultaneously topologically interconnected mesoporous network morphology, presence heteroatom species, lattice vibrational structure, complex interpretation requires need to supplement experimental observations theoretical calculations for further insights. The interplay pore size redox revealing distinctive supercapacitive (ion-adsorption controlled) pseudocapacitive (diffusion-controlled) energy storage mechanistic contributions arises from combined effects functional groups, most likely located on basal plane at edge sites. density theory provided band structure electron transfer Mulliken Hirshfeld population analyses helping discern nature various in diverse graphene. Interestingly, while quaternary (N—Q) pyridinic-N-oxides (N—O) planes capacitance due positive charge thus an higher current loads identified nitrogen-doped aerogel (AG/nitrogenated) GO-derived rGO chemical properties, other important affecting pyridinic (N-6) pyrrolic (N-5) nanosheet association carboxylic (—COOH) quinone (C=O) nitrogenated graphene/graphene coated polyaniline, contributing a character.