Organic electride C6O6Li6: A potential support for transition metal-doped single atom catalysis toward hydrogen evolution reaction (HER)

Abstract

In pursuit of efficient hydrogen evolution reaction (HER) catalysts, the use of single-atom catalysts (SACs) is crucial for the full realization of hydrogen energy. This study investigates the potential of the late first row transition metals (Fe – Zn) doped C₆O₆Li₆ organic electride as a support material towards HER. The intrinsic properties such as the geometry, stability, electronic properties, and HER catalytic activity of these SACs are assessed by employing the ωB97XD functional of the density functional theory (DFT) coupled with the def2TZVP basis-set. The Fe, Ni, and Co doped SACs show high stability, whereas Cu and Zn exhibit lower stability. The electronic properties analysis indicates sufficient conductivity for the designed SACs, as evidenced by their low E_gap values. Among the studied systems, Fe/Side@C₆O₆Li₆ SAC shows the best catalytic activity with a ΔG_H∗ value of −0.55 eV. Despite this, all studied systems demonstrate low HER activity. However, this study highlights the potential of organic electrides in catalytic applications and sets the groundwork for further optimization.