The Reactivity of Cobalt Clusters Con±/0 with Ammonia: Co3+ Cluster Catalysis for NH3 Dehydrogenation.
2020
The customized Re-TOF mass spectrometer combined with a 177-nm deep-ultraviolet laser has enabled us to observe well-resolved cobalt clusters Con±/0 and perform a comprehensive study on their reactivity with ammonia (NH3). The anions Con- are found to be inert, the neutrals allow to adsorb multiple NH3 molecules, while the cationic Con+ clusters readily react with NH3 giving rise to dehydrogenation. However, incidental dehydrogenation of NH3 on Con+ is only observed for n≥3. The dramatic charge- and size-dependent reactivities of Con±/0 clusters with NH3 are studied by the DFT-calculation results of energetics, density of states, orbital interactions, and reaction dynamics. We illustrate the dehydrogenation from two NH3 molecules, where a significantly reduced transition-state energy barrier is found pertaining to dimolecular co-catalysis effect. The reactivity of Co3+ with NH3 is illustrated showing effective catalysis for N-H dissociation to produce hydrogen applicable for designing ammonia fuel cells.
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