Thermal Dihydrogen Activation by a Closed-Shell AuCeO2(+) Cluster

Area of Science:

• Catalysis
• Surface Science
• Materials Chemistry

Background:

• Hydrogen activation is crucial for many chemical processes.
• Single-atom catalysis offers unique reactivity and selectivity.
• Metal oxide supports play a vital role in stabilizing active sites.

Purpose of the Study:

• To investigate the hydrogen activation mechanism on gold-cerium bimetallic oxide clusters.
• To compare the reactivity of AuCeO2(+) with CeO2(+) for H2 activation.
• To elucidate the role of single gold atoms in catalysis over oxide supports.

Main Methods:

• Laser ablation to generate AuCeO2(+) and CeO2(+) clusters.
• Mass selection using a quadrupole mass filter.
• Reaction with H2 in an ion trap reactor.
• Characterization by mass spectrometry and density functional theory (DFT) calculations.

Main Results:

• AuCeO2(+) clusters exhibit higher reactivity in H2 activation compared to CeO2(+) clusters.
• The gold atom acts as the primary active site for hydrogen adsorption.
• Heterolytic cleavage of H2 is facilitated by the gold atom and the oxide support.

Conclusions:

• This work presents the first instance of thermal H2 activation by a closed-shell atomic cluster.
• The findings provide molecular-level insights into single gold atom catalysis on metal oxide supports.
• This study highlights the potential of bimetallic oxide clusters for efficient hydrogen activation.