Dispersion-corrected DFT design of nitrogen doped- or TMN4 embedded buckybowl-like porous carbon derived from zeolitic imidazolate frameworks as anode material of sodium-ion battery

Porous carbon derived from Zeolitic Imidazolate Frameworks (ZIFs) has shown large surface area and high micropore volume making a promising electrode material for energy storage devices. In this research, pristine 3D C39H9 Buckybowl-like porous carbon (PC), nitrogen-doped PC (NPC), and both CoN4 and ZnN4-embedded PC (TMN4-PC) frameworks were designed by density function theory (DFT) were used as the anode in a sodium-ion battery (NIB). The calculations showed that the atomic and ionic sodium adsorption in the various frameworks maintained the semiconductor character. Also, bare PC, NPC, and TMN4-PC exhibited negative adsorption-energy values for the Na/Na+. Both Na+ and Na were preferably adsorbed on oxygenated NPC (o-NPC) and CoN4-NPC rather than the other surfaces where Na+ interacted better than Na. The cell voltage of the studied structures in the NIBs decreased in the following order: CoN4-NPC (0.81 V) > pyridinic-NPC (0.76 V) similar to edge graphitic-NPC (0.75 V) > basal plane graphitic-NPC (0.66 V) > basal plane pyrrolic-NPC (0.60 V) > edge pyrrolic-NPC (0.57 V) > bare PC (0.52 V) > ZnN4-NPC (0.50 V) >> o-NPC (0.36 V). The low Na-ion diffusion barriers on the surface of CoN4-NPC (0.10 eV) indicated a high potential for fast charge-discharge processes.

Automated summary

Porous carbon frameworks designed using DFT were studied as anodes for sodium-ion batteries, with the surface of CoN4-NPC showing a low sodium ion diffusion barrier, indicating potential for fast charge-discharge processes.