Transition-metal-atom anchored graphdiynes (TM@GDY, TM = Mn, Fe, Co, Ni and Cu) have already been synthesized and found applications in hydrogen evolution, nitrogen fixation and etc. By means of first-principle predictions and test experiments, we propose here that Fe@GDY and Co@GDY are efficient catalysts for the sustainable conversion of O3 to O2. These two catalysts can spontaneously chemisorb O3 with zero reaction barrier and have low O3 conversion barriers (0.31 eV and 0.19 eV, respectively). The O3 decomposition experiment in a continuous flow membrane reactor and electron paramagnetic resonance results verify that Fe@GDY and Co@GDY are efficient catalysts under humid conditions. Raman spectra prove the formation of the key Fe-O/Co-O and FeOO and CoOO intermediates. The hydrophobic nature of graphdiyne and the strongest chemisorption of O3 among tested ambient gases, make Fe@GDY and Co@GDY ideal catalysts under both dry and humid conditions. These findings would stimulate future explorations on metal anchored GDY-based catalysts for applications of toxic gas decomposition or fixation.
Keywords: Density functional theory; Metal anchored graphdiyne; Ozone decomposition; Surface reaction.
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