The distribution of methylcyclopentane (MCP) ring enlargement (RE) pro
ducts between benzene (Bz) and cyclohexane (Ch) provides information o
n the reaction mechanism. The Bz/CH ratio is in excess of the calculat
ed and experimentally determined equilibrium ratio. This implies that
benzene is a primary product; it eliminates the possibility of direct
hydride ion transfer to carbenium ions as the prevailing mechanism. Th
e results are consistent with the concept that metal-proton adducts ar
e instrumental in bifunctional catalysis.