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Thermal Dihydrogen Activation by a Closed-Shell AuCeO2+ Cluster

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posted on 2015-12-17, 05:35 authored by Jing-Heng Meng, Sheng-Gui He
Laser-ablation-generated AuCeO2+ and CeO2+ oxide clusters were mass-selected using a quadrupole mass filter and reacted with H2 in an ion trap reactor at ambient conditions. The reactions were characterized by mass spectrometry and density functional theory calculations. The gold–cerium bimetallic oxide cluster AuCeO2+ is more reactive in H2 activation than the pure cerium oxide cluster CeO2+. The gold atom is the active adsorption site and facilitates the heterolytic cleavage of H2 in collaboration with the separated O2– ion of the CeO2 support. To the best of our knowledge, this is the first example of thermal H2 activation by a closed-shell atomic cluster, which provides molecular-level insights into the single gold atom catalysis over metal oxide supports.