Abstract
Single-atom catalysts (SACs) are a new research frontier in electrocatalysis such as in the hydrogen evolution reaction (HER). Recent theoretical and experimental studies have demonstrated that certain M-N-C (metal-nitrogen-carbon) based SACs exhibit excellent performance for HER. Here we report a new approach to tune HER activity for SACs by changing the size and dimensionality of the carbon substrate while maintaining the same coordination environment. We screen the 3d, 4d, and 5d transition metal SACs in N-doped 2D graphene and nanographenes of several sizes for HER using first-principles density functional theory (DFT). Nanographenes containing V, Rh, and Ir are predicted to have significantly enhanced HER activity compared to their 2D graphene counterparts. We turn to machine learning to accurately predict the free energy of hydrogen adsorption (ΔGH) based on various descriptors and compressed sensing to identify key descriptors for activity, which can be used to further screen for additional candidates.
| Original language | English |
|---|---|
| Pages (from-to) | 19571-19578 |
| Number of pages | 8 |
| Journal | Journal of Physical Chemistry C |
| Volume | 124 |
| Issue number | 36 |
| DOIs | |
| State | Published - Sep 10 2020 |
Funding
This work was sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract DE-AC02-05CH11231.