Work on this project can be found at this repository: https://github.com/matthewkovacs/compreu
The immediate goal of this project would be to estimate trends of electron density of nitrogen across graphene sheets, with the focus of assessing the compound’s ability to catalyze reverse combustion. These polycyclic graphene compounds have shown affinity for CO2 but their ability to catalyze reverse combustion reactions, which will consume CO2 and produce hydrocarbon fuels, has yet to be evidenced. Previous experiments have shown the ability of pyrimidine to react with carbon dioxide in solution to produce formaldehyde.
By modeling the energies and geometries of the unbound lone pair electrons of nitrogen when localized in such graphene compounds, insight may be discovered with the overall goal of designing carbon nanofiber based methods of converting greenhouse gases into hydrocarbon fuels.
Density functional theory based single point energy calculations run by NWChem using B3LYP theory with 6-31G(d) basis and closed shell multiplicity of 1 assumptions, produced a total DFT energy of -2730.329563364568 Ha, exchange-correlation energy of -393.117967885533 Ha, Nuclear repulsion energy of 9710.099848810352 Ha, coulomb energy of 10993.192392458450 Ha, and one electron energy of -23040.503836747837 Ha. However, the NWChem calculation ran through 30 iterations without convergence and was terminated at the end of the thirtieth iteration with the above results.
Self-consistent field methods were also employed by Gaussian 09. Gaussian reported a value of -2730.32983435 A.U. after 27 cycles. An AM1 calculation was run by Ampac on the molecule above with the results of -9482.482466 eV or-348.4748184 Ha total energy, 6.864347 eV or 0.2522601 Ha ionization potential, and 3.716234 eV or 0.1365691 Ha HOMO-LUMO gap, after 53 SCF calculations. A series of Ampac calculation were performed on a sixty atom graphene sheet where each carbon atom was individually substituted for a nitrogen. A second series of energy calculations were run where the C-26 atom was substituted for a nitrogen and all other carbons were converted to nitrogens individually. The results of the calculations are described below, along with an index map of the carbon positions along the graphene sheet. A Pearson correlation between molecular energy and nitrogen position showed no correlation.