| AVS 66th International Symposium & Exhibition | |
| Fundamental Discoveries in Heterogeneous Catalysis Focus Topic | Friday Sessions |
| Session HC+SS-FrM |
| Session: | Catalysis at Complex Interfaces |
| Presenter: | Talat S. Rahman, University of Central Florida |
| Authors: | K.L. Chagoya, University of Central Florida T. Jiang, University of Central Florida D.J. Nash, University of Central Florida D. Le, University of Central Florida T.S. Rahman, University of Central Florida R.G. Blair, University of Central Florida |
| Correspondent: | Click to Email |
Finding effective heterogeneous catalysts, consisting of abundant elements, for the hydrogenation of waste gas carbon dioxide into value added molecules is a challenging task for global energy and sustainability solutions. In a closely coupled computational and experimental effort, we find that vacancies induced in defect-laden hexagonal boron nitride (dh-BN) can effectively activate the CO2 molecule for hydrogenation. Computationally, we demonstrate that activation occurs through back-donation to the π* orbitals of CO2 from frontier orbitals (defect state) of the h-BN sheet localized near a nitrogen vacancy (VN). Subsequent hydrogenation to formic acid (HCOOH) and methanol (CH3OH) occurs through vacancy facilitated co-adsorption of hydrogen and CO2. More importantly, we find that dh-BN is a temperature-driven switchable catalyst with formic acid formation observable at reaction temperatures above 160 ˚C and pressures of 583 kPa, while methanol formation was observed at lower temperatures (as low as 20 ˚C), which are in great agreement with thermodynamics and kinetics of our calculated reaction pathways.
*Work supported in part by DOE grant DE-FG02-07ER15842