Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 124, Issue 28, Pages 5879-5886Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.0c03720
Keywords
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Funding
- National Natural Science Foundation of China [91536105, 21722308, 21802146]
- CAS Key Research Project of Frontier Sciences (CAS) [QYZDB-SSW-SLH024]
- Frontier Cross Project of the National Laboratory for Molecular Sciences [051Z011BZ3]
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A customized reflection time-of-flight (Re-TOF) mass spectrometer combined with a 177 nm deep-ultraviolet laser has enabled us to observe well-resolved cobalt clusters Co-n(+/-/0) and perform a comprehensive study of their reactivity with ammonia (NH3). The anions Co-n(-) are found to be inert, the neutrals allow the adsorption of multiple NH3 molecules, while the cationic Co-n(+) clusters readily react with NH3 giving rise to dehydrogenation. However, incidental dehydrogenation of NH3 on Co-n(+) is only observed for n = 3. The dramatic charge- and size-dependent reactivities of Co-n(+/-/0) clusters with NH3 are studied by the density functional theory (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 the dimolecular co-catalysis effect. The reactivity of Co-3(+) with NH3 is illustrated showing effective catalysis for N-H dissociation to produce hydrogen applicable for designing ammonia fuel cells.
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