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Hydrogen adsorption on graphene-supported metal clusters has brought muchcontroversy due to the complex nature of the bonding between hydrogen and metalclusters. The bond types of hydrogen and graphene-supported Ti clusters areexperimentally and theoretically investigated. Transmission electron microscopyshows that Ti clusters of nanometer-size are formed on graphene. Thermaldesorption spectroscopy captures three hydrogen desorption peaks fromhydrogenated graphene-supported Ti clusters. First principle calculations alsofound three types of interaction: Two types of bonds with different partialionic character and physisorption. The physical origin for this rests on thecharge state of the Ti clusters: when Ti clusters are neutral, H2 isdissociated, and H forms bonds with the Ti cluster. On the other hand, H2 isadsorbed in molecular form on positively charged Ti clusters, resulting inphysisorption. Thus, this work clarifies the bonding mechanisms of hydrogen ongraphene-supported Ti clusters.

Revealing the multi-bonding state between hydrogen and graphene-supported Ti clusters