Methane Interactions with Heteroatom-Doped Carbon Surfaces

Rylan Rowsey, Erin E. Taylor, Stephan Irle, Nicholas P. Stadie, and Robert K. Szilagyi Department of Chemistry and Biochemistry, Montana State University, Bozeman, MT 59717 School of Chemical, Biological, and Environmental Engineering, Oregon State University, Corvallis, OR 97331

Methane storage by physisorption on a carbon-based surface is a well-established strategy; however, the effect of heteroatom inclusions, specifically boron and nitrogen, within the carbon surface remains unexplored. In this work, we employ various computational chemistry methods to investigate both structural and energetic effects on the approach of a methane molecule to the surface of a polyaromatic hydrocarbon molecule: 1-methylidenephenalene (MPh).  This molecule is selected for its aromaticity, low computational cost, and radial symmetry around a central atomic position that can be occupied by boron, carbon, or nitrogen. A suite of quantum chemical methods has been utilized, including density functional theory (MN15 functional) and wave function theory (MP2, CCSD(T), correlated post-Hartree-Fock methods) with a saturated all-electron basis set. Lowest energy structures of MPh and their heteroatom-doped derivatives have been obtained using the MN15 functional. Interaction energies between methane and the optimized MPh molecules have been assessed as a function of approach distance, angle, and location using a conceptually converging series of functionals ranging from MP2 up to CCSD(T), the most robust methods computationally accessible for us for the treatment of London dispersion forces. This work motivates important future synthetic strategies to substitutionally modify porous carbon adsorbent materials by heteroatom doping (especially by nitrogen) in order to strengthen methane binding and increase methane storage capacity at ambient temperature.

Additional Abstract Information

Presenter: Rylan Rowsey

Institution: Montana State University

Type: Poster

Subject: Chemistry

Status: Approved

Time and Location

Session: Poster 4
Date/Time: Tue 11:00am-12:00pm
Session Number: 3526