“…The electronic structures and physicochemical properties of transition metal oxides have been a subject of intense fundamental studies. − A prominent example is molybdenum oxide, on which extensive theoretical and experimental studies, ranging from small clusters to bulk structures of various phases, have been carried out. ,, Furthermore, hydrogen spillover phenomena have also been widely observed in the formation of hydrogen bronze materials in several transition metal oxides, for example, MoO 3 and WO 3 , since the early 70s. − The concept of hydrogen spillover was originated from studies of heterogeneous catalysis, − in which hydrogen bronze materials, such as H x MoO 3 , serve as catalysts for hydrogenation, dehydration, and reduction processes. The formation process and the structure of the compounds along with the associated catalytic activity and other properties have drawn considerable attention both experimentally and theoretically. − Furthermore, the efficiency of hydrogen spillover on metal oxides can be improved significantly in the presence of palladium and/or platinum catalysts . Solid-state 1 H NMR spectroscopy by Ritter and co-workers suggests that hydrogen atoms reside on a zigzag line connecting the vertex-sharing oxygen atoms of the intralayers of (MoO 6 ) n octahedra. , However, a recent combined theoretical and experimental study found no hydrogen occupation on the intralayer sites, even at high H atom concentrations .…”