Abstract
The intrinsic properties and catalytic performances of single- and double-transition metals on graphitic carbon nitride, TMn@g-C3N4 (n = 1,2), toward the O2 activation were investigated by DFT calculation. The 3d-TM atoms are firmly trapped inside g-C3N4 which prevents the metal clustering and shows high thermodynamic stability. The dimetal-dioxygen adsorption configuration of the O2/TM2@g-C3N4 promotes electron transfer from catalyst to the adsorbed O2, which improves their catalytic performances over the O2/TM@g-C3N4. We observed the two different electron transfer mechanisms for O2 activation on TMn@g-C3N4, in which the double-metal acts as an electron donor while the single-metal acts as the bridge for electron transfer from the substrate to the adsorbed O2. Remarkably, the catalytic performance of the TMn@g-C3N4 for O2 dissociation has a strong correlation with the three factors, (i) the charge gained on adsorbed O2, (ii) the O2 adsorption energy, and (iii) the O-O distance. The Fe2@g-C3N4 as a low-cost and non-precious metal catalyst shows the best catalytic performance with the lowest activation energy barrier of 0.26 eV for O2 activation, and therefore, is predicted as a potential catalyst for O2 consuming reactions. Our finding provides useful information for further design and development of high efficient few-atom catalysts based 2D-carbon materials.
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